Cha type zeolitic materials and methods for their preparation using combinations of cycloalkyl- and tetraalkylammonium compounds

ABSTRACT

The present invention relates to a process for the preparation of a zeolitic material having a CHA-type framework structure comprising YO 2  and X 2 O 3 , wherein said process comprises the steps of:
         (1) providing a mixture comprising one or more sources for YO 2 , one or more sources for X 2 O 3 , one or more tetraalkylammonium cation R 1 R 2 R 3 R 4 N + -containing compounds, and one or more tetraalkylammonium cation R 5 R 6 R 7 R 8 N + -containing compounds as structure directing agent;   (2) crystallizing the mixture obtained in step (1) for obtaining a zeolitic material having a CHA-type framework structure;       wherein Y is a tetravalent element and X is a trivalent element,   wherein R 1 , R 2 , R 3 , R 4 , R 5 , R 6 , and R 7  independently from one another stand for alkyl, and   wherein R 8  stands for cycloalkyl, as well as to zeolitic materials which may be obtained according to the inventive process and to their use.

TECHNICAL FIELD

The present invention relates to a process for the preparation of azeolitic material as well as to a zeolitic material having the CHA-typeframework structure as such and as obtainable from the inventiveprocess. Furthermore, the present invention relates to the use of theinventive zeolitic materials in specific applications.

Introduction

Molecular sieves are classified by the Structure Commission of theInternational Zeolite Association according to the rules of the IUPACCommission on Zeolite Nomenclature. According to this classification,framework-type zeolites and other crystalline microporous molecularsieves, for which a structure has been established, are assigned a threeletter code and are described in the Atlas of Zeolite Framework Types,5th edition, Elsevier, London, England (2001).

Among said zeolitic materials, Chabazite is a well studied example,wherein it is the classical representative of the class of zeoliticmaterials having a CHA framework structure. Besides aluminosilicatessuch as Chabazite, the class of zeolitic materials having a CHAframework structure comprises a large number of compounds furthercomprising phosphorous in the framework structure are known which areaccordingly referred to as silicoaluminophosphates (SAPO). In additionto said compounds, further molecular sieves of the CHA structure typeare known which contain aluminum and phosphorous in their framework, yetcontain little or no silica, and are accordingly referred to asaluminophosphates (APO). Zeolitic materials belonging to the class ofmolecular sieves having the CHA-type framework structure are employed ina variety of applications, and in particular serve as heterogeneouscatalysts in a wide range of reactions such as in methanol to olefincatalysis and selective catalytic reduction of nitrogen oxides NO_(x) toname some two of the most important applications. Zeolitic materials ofthe CHA framework type are characterized by three-dimensional8-membered-ring (8MR) pore/channel systems containing double-six-rings(D6R) and cages.

Zeolitic materials having a CHA-type framework structure and inparticular Chabazite with incorporated copper ions (Cu-CHA) are widelyused as heterogeneous catalyst for the selective catalytic reduction(SCR) of NO_(x) fractions in automotive emissions. Based on the smallpore openings and the alignment of the copper ions in the CHA cages,these catalyst systems have a unique thermal stability, which toleratestemperatures higher than 700° C. in presence of H₂O.

For the industrial production of CHA, cost intensive1-adamantyltriemethylammoniumhydroxid among other expensiveorganotemplates are typically employed as structure directing agent inthe synthetic procedures for their preparation. U.S. Pat. No. 4,544,538for example relates to the production of SSZ-13 using1N-alkyl-3-quinuclidinol, N,N,N-tetraalkyl-1-adamantammonium, orN,N,N-trialkyl-exo-aminonorbornane as the structure directing agent, theSSZ-13 zeolitic material having a CHA-type framework structure.

WO-A-2008/083048, on the other hand, concerns a method for theproduction of SSZ-13 using a specific N,N,N-trimethyl benzyl quaternaryammonium cation in the presence of seed crystals. Similarly,WO-A-2008/039742 relates to a method for the production of SSZ-13wherein a mixture of N,N,N-trialkyl benzyl quaternary ammonium cationsand N,N,N-tetramethyl-1-adamantammonium are employed as theorganotemplate in an effort for increasing cost-effectiveness byattempting to reduce the amount of the cost-intensiveN,N,N-tetramethyl-1-adamantammonium usually employed in the synthesis ofSSZ-13.

WO-A-2008/033229, concerns a method for the production of microporousmaterials using dicycloalkylammonium compounds as organic templatingagents.

WO 2009/141324 A1 relates to a method for the direct synthesis of Cucontaining Zeolites having the CHA framework structure, wherein saiddocument mentions N,N,N-trimethylcyclohexylammonium compounds amongseveral compounds as possible structure directing agents for obtaining azeolitic material having the CHA framework structure. Furthermore, saiddocument teaches the use of a 1-adamantyltrimethylammonium compound incombination with a further ammonium compound which may be atetramethylammonium compound.

WO 2011/064186 A1 and EP 2 325 143 A2, on the other hand, respectivelyrelate to a process for the preparation of zeolites having the CHAframework structure which employ tetramethylammonium hydroxide inaddition to at least one organic structure directing agent. Among thestructure directing agents which may be used to this effect, saiddocuments mention N,N,N-trimethylcyclohexylammonium compounds amongseveral compounds as possible structure directing agents for obtaining azeolitic material having the CHA framework structure, wherein howeverN,N,N-trimethyl-1-adamantyltrimethylammonium compounds are preferablyand effectively taught in said documents for obtaining theaforementioned material.

U.S. Pat. No. 4,610,854 discloses the use of trimethylcyclohexylammoniumfor the production of SSZ-15, which is a zeolitic material displaying aframework structure other than the CHA-type. US-A-2007/0043249, on theother hand, relates to the use of a group of tetraalkylammoniumcompounds including trimethylcyclohexylammonium as organotemplates forthe production of zeolitic materials having the CHA framework structure,wherein said materials are however restricted to alumino- orsilicoaluminophosphates necessarily containing P₂O₅ in their respectiveframeworks.

Zones et al. “A Study of Guest/Host Energetics for the Synthesis of CageStructures NON and CHA” in Studies in Surface Science and Catalysis,Vol. 84, pp. 29-36, Elsevier Science B. V. (1994) describes thesynthesis of SSZ-13 using a variety of organotemplates including thetrimethylcyclohexylammonium cation, wherein the latter would displayvery low rates of crystallization in particular when compared to the useof the adamantyltrimethylammonium cation. WO 2013/182974 A relates tothe use of trimethylcyclohexylammoniumhydroxide as organotemplate forthe synthesis of CHA-type zeolitic materials involving crystallizationtimes of 48 hours or more.

Consequently, there remains a need for a cost-effective process for theproduction of zeolitic materials having the CHA-type frameworkstructure. Furthermore, there is an ongoing need for improved zeoliticmaterials having the CHA-type framework structure, in particular withrespect to the catalytic properties for use in a variety of applicationand in particular for use in the treatment of NO_(x) in automotiveexhaust gas a catalyst and/or catalyst support. This applies inparticular in view of national legislation and environmental policywhich require increasing effectiveness of environmental catalysts suchas Cu-Chabazite and related zeolitic materials.

DETAILED DESCRIPTION

It was therefore the object of the present invention to provide animproved CHA-type zeolitic material, as well as to provide an improvedmethod for the production of such a catalyst, in particular in view ofcost-effectiveness. Thus it has surprisingly been found that an improvedCHA-type zeolite may be obtained by using specific combinations ofcycloalkylammonium compounds as organotemplates in the self-organizingsynthetic procedures typical of zeolite chemistry. Thus, it has quiteunexpectedly been found that besides providing an improved process forthe production of said zeolitic materials, in particular with respect tothe considerable increase in cost-effectiveness which may be achieved inview of the reduced reaction times necessary according to the inventiveprocess, the resulting zeolitic materials per se display highlyunexpected properties compared to the products of syntheses onlyemploying a cycloalkylammonium or other organic structure directingagent by itself. This applies not only with respect to the uniquephysical and chemical properties of the materials obtained according tothe inventive process but in particular with respect to their highlyunexpected catalytic properties, and more specifically in view of theiractivity in SCR catalytic applications.

Therefore, the present invention relates to a process for thepreparation of a zeolitic material having a CHA-type framework structurecomprising YO₂ and X₂O₃, wherein said process comprises the steps of:

-   -   (1) providing a mixture comprising one or more sources for YO₂,        one or more sources for X₂O₃, one or more tetraalkylammonium        cation R¹R²R³R⁴N⁺-containing compounds, and one or more        tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing compounds as        structure directing agent;    -   (2) crystallizing the mixture obtained in step (1) for obtaining        a zeolitic material having a CHA-type framework structure;

-   wherein Y is a tetravalent element and X is a trivalent element,

-   wherein R¹, R², R³, R⁴, R⁵, R⁶, and R⁷ independently from one    another stand for alkyl, and

-   wherein R⁸ stands for cycloalkyl.

Thus, it has surprisingly been found that by using a specificcombination of a cycloalkylammonium cation as structure directing agentand a tetraalkylammonium cation according to the inventive process, ahighly cost-effective process is provided, wherein even moreunexpectedly, said improved process actually leads to an improvedzeolitic material having the CHA-type framework structure compared tomaterials obtained by using the cycloalkylammonium cation by itself orother organotemplates either by themselves or in combination with atetraalkylammonium cation in their respective synthetic procedures. Thisis particularly apparent from the different physical and chemicalproperties obtained for the resulting materials which clearlydistinguish them from those known from the prior art, in particular inview of the surprisingly improved performance of the inventive catalystscompared to latter materials when used in SCR applications, whichconstitutes a highly important technical field in which CHA-typezeolitic materials are employed.

According to the present invention, it is preferred that in theinventive process, the mixture provided in step (1) does not contain anysubstantial amount of a source of Z₂O₅, wherein Z is P. Within themeaning of the present invention, the term “substantial” with respect tothe amount of a source for Z₂O₅ being contained in the mixture providedin step (1) and crystallized in step (2) according to particular andpreferred embodiments of the inventive process, this preferablyindicates an amount of 5 wt.-% or less of Z₂O₅ contained in a source forZ₂O₅ and based on 100 wt-% of YO₂ contained in the one or more sourcesfor YO₂, and more preferably indicates an amount of 1 wt.-% or less,more preferably of 0.5 wt.-% or less, more preferably of 0.1 wt.-% orless, more preferably of 0.05 wt.-% or less, more preferably of 0.01wt.-% or less, more preferably of 0.005 wt.-% or less, more preferablyof 0.001 wt.-% or less, more preferably of 0.0005 wt.-% or less, andeven more preferably of 0.0001 wt.-% or less of Z₂O₅ contained in asource for Z₂O₅ based on 100 wt-% of YO₂ contained in the one or moresources for YO₂.

According to the present invention it is further preferred that Z standsfor P and As, wherein more preferably Z is any pentavalent element whichis a source for Z₂O₅ in the CHR-framework structure crystallized in step(2).

According to the invention process, one or more sources for YO₂ areprovided in step (1), wherein said one or more sources may be providedin any conceivable form provided that a zeolitic material comprising YO₂and X₂O₃ and having the CHA-type framework structure is crystallized instep (2). Preferably, YO₂ is provided as such and/or has a compoundwhich comprises YO₂ as a chemical moiety and/or as a compound which(partly or entirely) is chemically transformed to YO₂ during theinventive process.

As regards YO₂ and/or precursors thereof employed in the inventiveprocess, there is no particular restriction as to the one or moreelements for which Y stands, provided that said element is a tetravalentelement and that it is comprised in the zeolitic material crystallizedin step (2). In particular, within the meaning of the present invention,YO₂ is at least partially and preferably entirely comprised in theframework structure of the zeolitic material as structure buildingelement, as opposed to non-framework elements which can be present inthe pores and cavities formed by the framework structure and typical forzeolitic materials in general. Thus, taking into account theaforementioned, Y may stand for any conceivable tetravalent element, Ystanding either for a single or several tetravalent elements. Preferredtetravalent elements according to the present invention include Si, Sn,Ti, Zr, Ge, as well as combinations of any two or more thereof.According to preferred embodiments of the present invention, Y standsfor Si and/or Sn, wherein according to particularly preferredembodiments of the present invention, Y comprises Si and even morepreferably Y is Si.

In preferred embodiments of the present invention, wherein Y stands forSi or for a combination of Si with one or more further tetravalentelements, the source for SiO₂ preferably provided in step (1) can alsobe any conceivable source. Thus, by way of example, any type of silicasand/or silicates and/or silica derivatives may be used, whereinpreferably the one or more sources for YO₂ comprises one or morecompounds selected from the group consisting of fumed silica, silicahydrosols, reactive amorphous solid silicas, silica gel, silicic acid,water glass, sodium metasilicate hydrate, sesquisilicate, disilicate,colloidal silica, pyrogenic silica, silicic acid esters, or mixtures ofany two or more of the afore-mentioned compounds may equally be used.According to particularly preferred embodiments, the one or more sourcesfor YO₂ used in step (1) of the inventive process are selected from thegroup consisting of fumed silica, silica hydrosols, reactive amorphoussolid silicas, silica gel, silicic acid, colloidal silica, silicic acidesters, and mixtures of two or more thereof. According to saidparticularly preferred embodiments, it is further preferred that the oneor more sources for YO₂ are selected from the group consisting of fumedsilica, silica hydrosols, reactive amorphous solid silicas, silica gel,colloidal silica, and mixtures of two or more thereof, wherein even morepreferably according to the inventive process, the one or more sourcesfor YO₂ comprises fumed silica and/or colloidal silica, preferablycolloidal silica.

Regarding the one or more tetraalkylammonium cations, R¹R²R³R⁴N⁺ furtherprovided in the mixture according to step (1) of the inventive process,there is no particular restriction as to the type and/or amount thereofprovided that R¹, R², R³, and R⁴ independently from one another standfor alkyl, provided that the type and/or amount thereof which isprovided in step (1) allows for the crystallization of a zeoliticmaterial having the CHA-type framework structure in step (2). Thus,regarding the alkyl moieties R¹, R², R³, and R⁴ of the one or moretetraalkylammonium cations R¹R²R³R⁴N⁺ provided in step (1) of theinventive process, these may, by way of example, independently from oneanother stand for optionally substituted and/or optionally branched(C₁-C₆)alkyl. According to the present invention, R¹, R², R³, and R⁴ maybe the same, or two of R¹, R², R³, and R⁴ may be the same and onedifferent from the others, or R¹, R², R³, and R⁴ may each be differentfrom one another, wherein it is preferred that at least two of R¹, R²,R³, and R⁴ are the same alkyl moiety, and more preferably at least threeof R¹, R², R³, and R⁴ are the same alkyl moiety, and wherein even morepreferably R¹, R², R³, and R⁴ are the same alkyl moiety according toparticular embodiments of the present invention. As regards preferredembodiments of the present invention, R¹, R², R³, and R⁴ independentlyfrom one another stand for optionally substituted and/or optionallybranched (C₁-C₅)alkyl, wherein more preferably R¹, R², R³, and R⁴ areindependently from one another selected from the group consisting of(C₁-C₄)alkyl, more preferably (C₁-C₃)alkyl, wherein even more preferablyR¹, R², R³, and R⁴ independently form one another stand for optionallysubstituted methyl or ethyl. According to particularly preferredembodiments of the present invention, at least one, preferably two, morepreferably three, and even more preferably all of R¹, R², R³, and R⁴stand for optionally substituted methyl, preferably for unsubstitutedmethyl.

Therefore, as concerns the one or more tetraalkylammonium cationsR¹R²R³R⁴N⁺ further provided in the mixture according to step (1) of theinventive process, it is preferred according to the present inventionthat R¹, R², R³, and R⁴ independently from one another stand foroptionally substituted and/or optionally branched (C₁-C₆)alkyl,preferably (C₁-C₅)alkyl, more preferably (C₁-C₄)alkyl, more preferably(C₁-C₃)alkyl, and even more preferably for optionally substituted methylor ethyl, wherein even more preferably R¹, R², R³, and R⁴ stand foroptionally substituted methyl, preferably unsubstituted methyl.

Furthermore, it is preferred according to the inventive process that theone or more tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compoundscomprise one or compounds selected from the group consisting oftetra(C₁-C₆)alkylammonium compounds, preferablytetra(C₁-C₅)alkylammonium compounds, more preferablytetra(C₁-C₄)alkylammonium compounds, and more preferablytetra(C₁-C₃)alkylammonium compounds, wherein independently from oneanother the alkyl substituents are optionally substituted and/oroptionally branched. More preferably, the one or more tetraalkylammoniumcation R¹R²R³R⁴N⁺-containing compounds are selected from the groupconsisting of optionally substituted and/or optionally branchedtetrapropylammonium compounds, ethyltripropylammonium compounds,diethyldipropylammonium compounds, triethylpropylammonium compounds,methyltripropylammonium compounds, dimethyldipropylammonium compounds,trimethylpropylammonium compounds, tetraethylammonium compounds,triethylmethylammonium compounds, diethyldimethylammonium compounds,ethyltrimethylammonium compounds, tetramethylammonium compounds, andmixtures of two or more thereof, and preferably from the groupconsisting of optionally substituted and/or optionally branchedtetraethylammonium compounds, triethylmethylammonium compounds,diethyldimethylammonium compounds, ethyltrimethylammonium compounds,tetramethylammonium compounds, and mixtures of two or more thereof.According to the present invention it is particularly preferred that theone or more tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compoundsare selected from the group consisting of optionally substitutedtetramethylammonium compounds, wherein more preferably the one or moretetraalkylammonium cation R¹R²R³R⁴R⁺-containing compounds comprises oneor more tetramethylammonium compounds, and wherein more preferably theone or more tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compoundsconsists of one or more tetramethylammonium compounds.

According to the present invention, there is no particular restrictionas to the type of the one or more tetraalkylammonium cationsR¹R²R³R⁴N⁺-containing compounds which may be provided in step (1) of theinventive process provided that the one or more tetraalkylammoniumcations R¹R²R³R⁴N⁺ contained therein may act as structure directingagent upon crystallization of the reaction mixture in step (2) of theinventive process. According to preferred embodiments, the one or moretetraalkylammonium cations R¹R²R³R⁴N⁺-containing compounds contain oneor more salts. In principle, according to said preferred embodiments,there is no particular restriction as to the counter ion to the one ormore tetraalkylammonium cations R¹R²R³R⁴N⁺, again provided that theseallow for the crystallization of a zeolitic material having a CHA-typeframework structure in step (2) of the inventive process by thestructure directing action of one or more of the aforementionedtetraalkylammonium cations R¹R²R³R⁴N⁺. Thus, by way of example, the oneor more tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compounds maycomprise one or more salts selected from halides, hydroxides, sulfates,nitrates, phosphates, acetates, and mixtures of two or more thereof. Asregards the halide salts, these are preferably chloride and/or bromidesalts, wherein even more preferably chloride salts are employed.According to preferred embodiments of the present invention, the one ormore tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compounds compriseone or more one of more salts selected from the group consisting ofchlorides, hydroxides, sulfates, and mixtures of two or more thereof,wherein more preferably the one or more tetraalkylammonium cationR¹R²R³R⁴N⁺-containing compounds are tetraalkylammonium hydroxides and/orchlorides. According to particularly preferred embodiments, the one ormore tetraalkylammonium cations R¹R²R³R⁴N⁺-containing compounds areprovided as their hydroxide salts in step (1) of the inventive process.

Thus, according to particularly preferred embodiments of the inventiveprocess which are further preferred, the one or more tetraalkylammoniumcation R¹R²R³R⁴N⁺-containing compounds provided in step (1) comprise oneor more compounds selected from the group consisting oftetra(C₁-C₆)alkylammonium hydroxides, preferablytetra(C₁-C₅)alkylammonium hydroxides, more preferablytetra(C₁-C₄)alkylammonium hydroxides, and more preferablytetra(C₁-C₃)alkylammonium hydroxides, wherein independently from oneanother the alkyl substituents are optionally substituted and/oroptionally branched, wherein it is further preferred that the one ormore tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compounds isselected from the group consisting of optionally substituted and/oroptionally branched tetrapropylammonium hydroxide,ethyltripropylammonium hydroxide, diethyldipropylammonium hydroxide,triethylpropylammonium hydroxide, methyltripropylammonium hydroxide,dimethyldipropylammonium hydroxide, trimethylpropylammonium hydroxide,tetraethylammonium hydroxide, triethylmethylammonium hydroxide,diethyldimethylammonium hydroxide, ethyltrimethylammonium hydroxide,tetramethylammonium hydroxide, and mixtures of two or more thereof. Itis yet further preferred that the one or more tetraalkylammonium cationR¹R²R³R⁴N⁺-containing compounds is selected from the group consisting ofoptionally substituted and/or optionally branched tetraethylammoniumhydroxide, triethylmethylammonium hydroxide, diethyldimethylammoniumhydroxide, ethyltrimethylammonium hydroxide, tetramethylammoniumhydroxide, and mixtures of two or more thereof. According to embodimentsof the present invention which are even further preferred, the one ormore tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compounds compriseoptionally substituted tetramethylammonium hydroxide, wherein even morepreferably the tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compoundprovided in step (1) is tetramethylammonium hydroxide.

Regarding the one or more tetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺ furtherprovided in the mixture according to step (1) of the inventive process,there is no particular restriction as to the type and/or amount thereofprovided that R⁵, R⁶, and R⁷ independently from one another stand foralkyl and R⁸ stands for a cycloalkyl moiety, provided that the typeand/or amount thereof which is provided in step (1) allows for thecrystallization of a zeolitic material having the CHA-type frameworkstructure in step (2). Thus, regarding the alkyl moieties R⁵, R⁶, and R⁷of the one or more tetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺ provided instep (1) of the inventive process, these may, by way of example,independently from one another stand for optionally substituted and/oroptionally branched (C₁-C₆)alkyl. According to the present invention,R⁵, R⁶, and R⁷ may be the same, or two of R⁵, R⁶, and R⁷ may be the sameand one different from the others, or R⁵, R⁶, and R⁷ may each bedifferent from one another, wherein it is preferred that at least two ofR⁵, R⁶, and R⁷ are the same alkyl moiety, and wherein even morepreferably R⁵, R⁶, and R⁷ are the same alkyl moiety according toparticular embodiments of the present invention. As regards preferredembodiments of the present invention, R⁵, R⁶, and R⁷ independently fromone another stand for optionally substituted and/or optionally branched(C₁-C₅)alkyl, wherein more preferably R⁵, R⁶, and R⁷ are independentlyfrom one another selected from the group consisting of (C₁-C₄)alkyl,more preferably (C₁-C₃)alkyl, wherein even more preferably R⁵, R⁶, andR⁷ independently form one another stand for optionally substitutedmethyl or ethyl. According to particularly preferred embodiments of thepresent invention, at least one, preferably two, and even morepreferably all of R⁵, R⁶, and R⁷ stand for optionally substitutedmethyl, preferably for unsubstituted methyl.

Therefore, as concerns the one or more tetraalkylammonium cationsR⁵R⁶R⁷R⁸N⁺ further provided in the mixture according to step (1) of theinventive process, it is preferred according to the present inventionthat R⁵, R⁶, and R⁷ independently from one another stand for optionallysubstituted and/or optionally branched (C₁-C₆)alkyl, preferably(C₁-C₅)alkyl, more preferably (C₁-C₄)alkyl, more preferably(C₁-C₃)alkyl, and even more preferably for optionally substituted methylor ethyl, wherein even more preferably R⁵, R⁶, and R⁷ stand foroptionally substituted methyl, preferably unsubstituted methyl.

As regards the cycloalkyl moiety R⁸ of the one or moretetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺ provided in step (1) of theinventive process, R⁸ may stand for any suitable cycloalkyl group and ispreferably cycloalkyl selected from the group consisting optionallyheterocyclic and/or optionally substituted cycloalkyl. As regards thenumber of chain members forming the optionally heterocyclic cycloalkylmoiety, no particular restriction applies in this respect according tothe present invention, provided that a zeolitic material having aCHA-type framework structure may be crystallized in step (2) of theinventive process. Thus, by way of example, the optionally heterocycliccycloalkyl moiety may be formed from any suitable number of chainmembers, wherein it is preferred that the ring moiety is formed fromoptionally heterocyclic 5- to 8-membered cycloalkyl, more preferably 5-to 7-membered cycloalkyl, more preferably 5- or 6-membered cycloalkyl,wherein even more preferably the optionally heterocyclic cycloalkyl is a6-membered cycloalkyl. As regards the moieties by which the optionallyheterocyclic cycloalkyl moieties according to the present invention maybe substituted, there is again no particular restriction in this respectprovided that a zeolitic material having a CHA-type framework structuremay be crystallized in step (2). Thus, by way of example, the one ormore optional substituents of the optionally heterocyclic moiety may beselected from the group consisting of (C₁-C₃)alkyl, (C₁-C₃)alkoxy,hydroxyl, halides, (C₁-C₃)carboxyl, (C₁-C₃)carbonyl, (C₁-C₃)amine andcombinations of two or more thereof, preferably from the groupconsisting of (C₁-C₂)alkyl, (C₁-C₂)alkoxy, hydroxyl, chloro, bromo,fluoro, and combinations of two or more thereof, more preferably fromthe group consisting of methyl, hydroxyl, chloro, and combinations oftwo or more thereof, wherein even more preferably the one or moreoptional substituents is methyl and/or hydroxo, preferably methyl. Asregards the number of substituents which are present on the optionallyheterocyclic cycloalkyl moiety according to particular embodiments ofthe present invention, their number may range anywhere from 1 to 4,wherein preferably from 1 to 3 substituents are present on theoptionally heterocyclic cycloalky, more preferably 1 or 2, wherein evenmore preferably one substituent is present on the optionally heterocyliccycloalkyl moiety of R⁸ according to particular embodiments of thepresent invention. According to the present invention, it is howeverparticularly preferred that R⁸ stands for optionally heterocycliccycloalkyl which is unsubstituted, and even more preferably forcyclohexyl.

Regarding the heteroatom which may be present in embodiments of thepresent invention wherein R⁸ is an optionally substituted heterocycliccycloalkyl, no particular restriction applies according to the presentinvention, neither with respect to the type of heteroatoms which may bepresent in the heterocyclic cycloalkyl moiety, nor with respect to theirnumber, provided that a zeolitic material having the CHA-type frameworkstructure may be crystallized in step (2). Thus, by way of example, theone or more heteroatoms comprised in the heterocyclic cycloalkyl maycomprise one or more elements selected from the group consisting of N,O, S, Se, P, Cl, Br, I, and combinations of two or more thereof, whereinpreferably the one or more heteroatoms comprise one or more elementsselected from the group consisting of N, O, S, Se, P, and combinationsof two or more thereof, more preferably from the group consisting of N,O, S, and combinations of two or three thereof, wherein even morepreferably the one or more heteroatoms comprise N and/or O, preferablyO. As regards the number of heteroatoms which are contained as chainmembers of the heterocyclic cycloalkyl according to particularembodiments of the present invention, their number may range anywherefrom 1 to 4, wherein preferably from 1 to 3 heteroatoms are present inthe heterocyclic cycloalky, more preferably 1 or 2, wherein even morepreferably one heteroatom is contained in the heterocylic cycloalkylmoiety of R⁸ according to particular embodiments of the presentinvention. It is, however, particularly preferred according to thepresent invention that the cycloalkyl moiety R⁸ of the one or moretetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing compounds provided instep (1) of the inventive process is cycloalkyl which does not contain aheteroatom, preferably cyclohexyl.

Therefore, as concerns the one or more tetraalkylammonium cationsR⁵R⁶R⁷R⁸N⁺ further provided in the mixture according to step (1) of theinventive process, it is preferred according to the present inventionthat R⁸ stands for optionally heterocyclic and/or optionally substituted5- to 8-membered cycloalkyl, preferably for 5- to 7-membered cycloalkyl,more preferably for 5- or 6-membered cycloalkyl, wherein even morepreferably R⁸ stands for optionally heterocyclic and/or optionallysubstituted 6-membered cycloalkyl, preferably optionally substitutedcyclohexyl, and more preferably non-substituted cyclohexyl.

Furthermore, according to particularly preferred embodiments of theinventive process, the one or more tetraalkylammonium cationR⁵R⁶R⁷R⁸N⁺-containing compounds comprise one or moreN,N,N-tri(C₁-C₄)alkyl-(C₅-C₇)cycloalkylammonium compounds, preferablyone or more N,N,N-tri(C₁-C₃)alkyl-(C₅-C₆)cycloalkylammonium compounds,more preferably one or moreN,N,N-tri(C₁-C₂)alkyl-(C₅-C₆)cycloalkylammonium compounds, morepreferably one or more N,N,N-tri(C₁-C₂)alkyl-cyclopentylammonium and/orone or more N,N,N-tri(C₁-C₂)alkyl-cyclohexylammonium compounds, morepreferably one or more compounds selected fromN,N,N-triethyl-cyclohexylammonium,N,N-diethyl-N-methyl-cyclohexylammonium,N,N-dimethyl-N-ethyl-cyclohexylammonium,N,N,N-trimethyl-cyclohexylammonium compounds, and mixtures of two ormore thereof, wherein it is even more preferred according to theinventive process that the one or more tetraalkylammonium cationR⁵R⁶R⁷R⁸N⁺-containing compounds comprise one or moreN,N,N-trimethyl-cyclohexylammonium compounds, wherein it is even furtherpreferred that the one or more tetraalkylammonium cationR⁵R⁶R⁷R⁸N⁺-containing compounds provided in step (1) of the inventiveprocess consists of one or more N,N,N-trimethyl-cyclohexylammoniumcompounds, even more preferably of a singleN,N,N-trimethyl-cyclohexylammonium compound.

According to the present invention, there is no particular restrictionas to the type of the one or more tetraalkylammonium cationsR⁵R⁶R⁷R⁸N⁺-containing compounds which may be provided in step (1) of theinventive process provided that the one or more tetraalkylammoniumcations R⁵R⁶R⁷R⁸N⁺ contained therein may act as structure directingagent upon crystallization of the reaction mixture in step (2) of theinventive process. According to preferred embodiments, the one or moretetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺-containing compounds contain oneor more salts. In principle, according to said preferred embodiments,there is no particular restriction as to the counter ion to the one ormore tetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺, again provided that theseallow for the crystallization of a zeolitic material having a CHA-typeframework structure in step (2) of the inventive process by thestructure directing action of one or more of the aforementionedtetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺. Thus, by way of example, the oneor more tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing compounds maycomprise one or more salts selected from halides, hydroxides, sulfates,nitrates, phosphates, acetates, and mixtures of two or more thereof. Asregards the halide salts, these are preferably chloride and/or bromidesalts, wherein even more preferably chloride salts are employed.According to preferred embodiments of the present invention, the one ormore tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing compounds compriseone or more one of more salts selected from the group consisting ofchlorides, hydroxides, sulfates, and mixtures of two or more thereof,wherein more preferably the one or more tetraalkylammonium cationR⁵R⁶R⁷R⁸N⁺-containing compounds are tetraalkylammonium hydroxides and/orchlorides. According to particularly preferred embodiments, the one ormore tetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺-containing compounds areprovided as their hydroxide salts in step (1) of the inventive process.

Thus, according to particularly preferred embodiments of the inventiveprocess which are further preferred, the one or more tetraalkylammoniumcation R⁵R⁶R⁷R⁸N⁺-containing compounds provided in step (1) comprise oneor more compounds selected from the group consisting ofN,N,N-tri(C₁-C₄)alkyl-(C₅-C₇)cycloalkylammonium hydroxides, preferablyof N,N,N-tri(C₁-C₃)alkyl-(C₅-C₆)cycloalkylammonium hydroxides, morepreferably of N,N,N-tri(C₁-C₂)alkyl-(C₅-C₆)cycloalkylammoniumhydroxides, more preferably of N,N,N-tri(C₁-C₂)alkyl-cyclopentylammoniumand/or N,N,N-tri(C₁-C₂)alkyl-cyclohexylammonium hydroxides, wherein itis yet further preferred that the one or more tetraalkylammonium cationR⁵R⁶R⁷R⁸N⁺-containing compounds is selected from the group consisting ofN,N,N-triethyl-cyclohexylammonium hydroxide,N,N-diethyl-N-methyl-cyclohexylammonium hydroxide,N,N-dimethyl-N-ethyl-cyclohexylammonium hydroxide,N,N,N-trimethyl-cyclohexylammonium hydroxide, and mixtures of two ormore thereof. According to embodiments of the present invention whichare even further preferred, the one or more tetraalkylammonium cationR⁵R⁶R⁷R⁸N⁺-containing compounds compriseN,N,N-trimethyl-cyclohexylammonium hydroxide, wherein even morepreferably the tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing compoundprovided in step (1) is N,N,N-trimethyl-cyclohexylammonium hydroxide.

According to the present invention the mixture provided in step (1)further comprises one or more sources for X₂O₃, wherein X is a trivalentelement. As regards the elements which may be employed as the trivalentelement X comprised in the one or more sources for X₂O₃ provided in step(1), there is no particular restriction according to the presentinvention as to which elements or element mixtures may be employed,provided that a zeolitic material having a CHA-type framework structureis crystallized in step (2) comprising YO₂ and X₂O₃ as frameworkelements. According to preferred embodiments of the present invention, Xis selected from the group consisting of Al, B, In, Ga, and mixtures oftwo or more thereof, wherein preferably X is Al and/or B. According toparticularly preferred embodiments of the present invention, X comprisesAl, wherein even more preferably X is Al.

According to the present invention, the mixture provided in step (1)comprises one or more sources for X₂O₃. In instances wherein one or moresources of Al₂O₃ is contained in the mixture, it is preferred that saidone or more sources comprises one or more compounds selected from thegroup consisting of alumina, aluminates, aluminum salts, and mixtures oftwo or more thereof, wherein the aluminates are preferably one or morealuminate salts selected from the group consisting of alkaline metalaluminates, aluminum hydroxide, and mixtures of two or more thereof, thealkaline metal preferably being sodium and/or potassium, and morepreferably being sodium. According to the present invention it isfurther preferred that the one or more sources or X₂O₃ comprise one ormore compounds selected from the group consisting of alumina, aluminumsalts, and mixtures of two or more thereof, wherein more preferably theone or more sources for X₂O₃ are selected from the group consisting ofalumina, aluminum tri(C₁-C₅)alkoxide, AlO(OH), Al(OH)₃, aluminumhalides, and mixtures of two or more thereof, wherein the aluminumhalides are preferably aluminum chloride and/or chloride and/or bromide,more preferably aluminum fluoride and/or chloride, and even morepreferably aluminum chloride. It is yet further preferred that the oneor more sources for X₂O₃ comprise one or more compounds selected fromthe group consisting of aluminum chloride, aluminum sulfate, aluminumphosphate, aluminum fluorosilicate, and mixtures of two or more thereof,wherein more preferably the one or more sources for X₂O₃ comprise one ormore compounds selected from the group consisting of aluminumtri(C₂-C₄)alkoxide, AlO(OH), Al(OH)₃, aluminum chloride, aluminumsulfate, aluminum phosphate, and mixtures of two or more thereof. It isparticularly preferred according to the present invention that the oneor more sources for X₂O₃ comprise one or more compounds selected fromthe group consisting of aluminum tri(C₂-C₃)alkoxide, AlO(OH), Al(OH)₃,aluminum chloride, aluminum sulfate, and mixtures of two or morethereof, more preferably from the group consisting of aluminumtripropoxides, AlO(OH), aluminum sulfate, and mixtures of two or morethereof, wherein more preferably the one or more sources for X₂O₃comprises aluminum triisopropoxide, and wherein even more preferably theone or more sources for X₂O₃ consists of aluminum triisopropoxide.

In step (1) according to the present invention, the mixture can beprepared by any conceivable means, wherein mixing by agitation ispreferred, preferably by means of stirring.

In preferred embodiments of the inventive process, the mixture providedin step (1) further comprises one or more solvents. According to theinventive process, there is no particular restriction whatsoever neitherwith respect to the type and/or number of the one or more solvents, norwith respect to the amount in which they may be used in the inventiveprocess provided that a zeolitic material having the CHA-type frameworkstructure may be crystallized in step (2). According to the inventiveprocess it is however preferred that the one or more solvents comprisewater, and more preferably distilled water, wherein according toparticularly preferred embodiments distilled water is used as the onlysolvent in the mixture provided in step (1).

In preferred embodiments of the inventive process wherein one or moresolvents are employed, there is no particular restriction as to theamount in which they may be used, wherein in particularly preferredembodiments employing water and more preferably distilled water, theH₂O:YO₂ molar ratio of the mixture may range by way of example anywherefrom 1 to 50, wherein preferably the molar ratio employed is comprisedin the range of from 3 to 30, more preferably of from 5 to 25, morepreferably of from 7 to 20, and even more preferably of from 9 to 17.According to particularly preferred embodiments of the present inventionwherein water and preferably distilled water is comprised among the oneor more solvents provided in step (1) and even more preferably is thesole solvent used in the reaction mixture crystallized in step (2), theH₂O:YO₂ molar ratio is comprised in the range of from 11 to 15.

As regards the amount in which the one or more tetraalkylammoniumcations R¹R²R³R⁴N⁺ may be provided in the mixture in step (1) of theinventive process, no particular restriction applies provided that azeolitic material having a CHA-type framework structure may becrystallized in step (2) of the inventive process. Thus, by way ofexample, the molar ratio of the one or more tetraalkylammonium cationsR¹R²R³R⁴N⁺:YO₂ provided in the mixture may range anywhere from 0.005 to0.5, wherein preferably the molar ratio is comprised in the range offrom 0.01 to 0.25, more preferably from 0.03 to 0.2, more preferablyfrom 0.05 to 0.15, more preferably from 0.07 to 0.12, and morepreferably from 0.08 to 0.11, According to particularly preferredembodiments of the present invention, the molar ratio of the one or moretetraalkylammonium cations R¹R²R³R⁴N⁺:YO₂ provided in the mixtureaccording to step (1) is comprised in the range of from 0.085 to 0.10.

Same applies accordingly relative to the amount in which the one or moretetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺ may be provided in the mixture instep (1) of the inventive process, such that no particular restrictionapplies in this respect as well, provided that a zeolitic materialhaving a CHA-type framework structure may be crystallized in step (2) ofthe inventive process. Thus, by way of example, the molar ratio of theone or more tetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺:YO₂ provided in themixture may range anywhere from 0.001 to 2.0, wherein preferably themolar ratio is comprised in the range of from 0.005 to 1.0, morepreferably from 0.01 to 0.5, more preferably from 0.03 to 0.3, morepreferably from 0.05 to 0.25, more preferably from 0.07 to 0.22, morepreferably from 0.08 to 0.2, and more preferably from 0.09 to 0.19.According to particularly preferred embodiments of the presentinvention, the molar ratio of the one or more tetraalkylammonium cationsR⁵R⁶R⁷R⁸N⁺:YO₂ provided in the mixture according to step (1) iscomprised in the range of from 0.10 to 0.18.

Concerning the relative amounts of the one or more tetraalkylammoniumcations R¹R²R³R⁴N⁺ and R⁵R⁶R⁷R⁸N⁺ to one another, these may be used inany suitable relation to one another provided that a CHA-type frameworkstructure may be crystallized in step (2) of the inventive process.Thus, with respect to the molar ratio R¹R²R³R⁴N⁺:R⁵R⁶R⁷R⁸N⁺ of the oneor more tetraalkylammonium cations R¹R²R³R⁴N⁺ and the one or moretetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺ contained in the mixture providedaccording to step (1), no particular restriction applies such that, byway of example, the molar ratio R¹R²R³R⁴N⁺:R⁵R⁶R⁷R⁸N⁺ may range anywherefrom 0.01 to 5, wherein preferably the molar ratio is comprised in therange of from 0.05 to 2, more preferably from 0.1 to 1.5, morepreferably from 0.2 to 1.2, more preferably from 0.3 to 1.1, morepreferably from 0.4 to 1, and more preferably from 0.45 to 0.65.According to the present invention, it is particularly preferred thatthe molar ratio R¹R²R³R⁴N⁺:R⁵R⁶R⁷R⁸N⁺ in the mixture provided accordingto step (1) is comprised in the range of from 0.5 to 0.9.

As regards the crystallization performed in step (2) of the inventiveprocess, no particular restriction applies according to the presentinvention as to the actual means employed for allowing thecrystallization of a zeolitic material from the mixture of step (1).Thus, any suitable means may be employed wherein it is preferred thatthe crystallization is achieved by heating of the mixture of step (1).According to said preferred embodiments, no particular restriction againapplies with respect to the temperature at which said crystallizationmay be achieved, wherein it is preferred that the crystallization isconducted under heating at a temperature comprised in the range of from90 to 250° C., more preferably of from 100 to 220° C., more preferablyfrom 130 to 200° C., more preferably from 150 to 190° C., and morepreferably from 160 to 180° C. According to the present invention it isparticularly preferred that the preferred heating of the mixtureprovided in step (1) in step (2) for the crystallization of a zeoliticmaterial is conducted at a temperature comprised in the range of from165 to 175° C.

Concerning the heating preferably employed in step (2) of the inventiveprocess as means for the crystallization of the zeolitic material, saidheating may in principle be conducted under any suitable pressureprovided that crystallization is achieved. In preferred embodiments ofthe present invention, the mixture according to step (1) is subjected instep (2) to a pressure which is elevated with regard to normal pressure.The term “normal pressure” as used in the context of the presentinvention relates to a pressure of 101,325 Pa in the ideal case.However, this pressure may vary within boundaries known to the personskilled in the art. By way of example, this pressure can be in the rangeof from 95,000 to 106,000 or of from 96,000 to 105,000 or of from 97,000to 104,000 or of from 98,000 to 103,000 or of from 99,000 to 102,000 Pa.

In preferred embodiments of the inventive process wherein a solvent ispresent in the mixture according to step (1), it is furthermorepreferred that heating in step (2) is conducted under solvothermalconditions, meaning that the mixture is crystallized under autogenouspressure of the solvent which is used, for example by conducting heatingin an autoclave or other crystallization vessel suited for generatingsolvothermal conditions. In particularly preferred embodiments whereinthe solvent comprises water, preferably distilled water, heating in step(2) is accordingly preferably conducted under hydrothermal conditions.

The apparatus which can be used in the present invention forcrystallization is not particularly restricted, provided that thedesired parameters for the crystallization process can be realized, inparticular with respect to the preferred embodiments requiringparticular crystallization conditions. In the preferred embodimentsconducted under solvothermal conditions, and in particular underhydrothermal conditions, any type of autoclave or digestion vessel canbe used.

Furthermore, as regards the period in which the preferred heating instep (2) of the inventive process is conducted for crystallizing thezeolitic material, there is again no particular restriction in thisrespect, provided that the period of heating is suitable for achievingcrystallization. Thus, by way of example, the period of heating mayrange anywhere from 3 to 40 h, preferably from 5 to 30 h, morepreferably from 8 to 25 h, more preferably from 10 to 22 h, and morepreferably from 13 to 21 h. According to the present invention it isparticularly preferred that heating in step (2) of the inventive processis conducted for a period of from 15 to 20 h.

According to preferred embodiments of the present invention, wherein themixture is heated in step (2), said heating may be conducted during theentire crystallization process or during only one or more portionsthereof, provided that a zeolitic material is crystallized. Preferably,heating is conducted during the entire duration of crystallization.

Further regarding the means of crystallization in step (2) of theinventive process, it is principally possible according to the presentinvention to perform said crystallization either under static conditionsor by means of agitating the mixture. According to embodiments involvingthe agitation of the mixture, there is no particular restriction as tothe means by which said agitation may be performed such that any one ofvibrational means, rotation of the reaction vessel, and/or mechanicalstirring of the reaction mixture may be employed to this effect whereinaccording to said embodiments it is preferred that agitation is achievedby stirring of the reaction mixture. According to alternativelypreferred embodiments, however, crystallization is performed understatic conditions, i.e. in the absence of any particular means ofagitation during the crystallization process.

In general, the process of the present invention can optionally comprisefurther steps for the work-up and/or further physical and/or chemicaltransformation of the zeolitic material crystallized in step (2) fromthe mixture provided in step (1). The crystallized material can forexample be subject to any sequence of isolation and/or washingprocedures, wherein the zeolitic material obtained from crystallizationin step (2) is preferably subject to at least one isolation and at leastone washing procedure.

Isolation of the crystallized product can be achieved by any conceivablemeans. Preferably, isolation of the crystallized product can be achievedby means of filtration, ultrafiltration, diafiltration, centrifugationand/or decantation methods, wherein filtration methods can involvesuction and/or pressure filtration steps.

With respect to one or more optional washing procedures, any conceivablesolvent can be used. Washing agents which may be used are, for example,water, alcohols, such as methanol, ethanol or propanol, or mixtures oftwo or more thereof. Examples of mixtures are mixtures of two or morealcohols, such as methanol and ethanol or methanol and propanol orethanol and propanol or methanol and ethanol and propanol, or mixturesof water and at least one alcohol, such as water and methanol or waterand ethanol or water and propanol or water and methanol and ethanol orwater and methanol and propanol or water and ethanol and propanol orwater and methanol and ethanol and propanol. Water or a mixture of waterand at least one alcohol, preferably water and ethanol, is preferred,distilled water being very particularly preferred as the only washingagent.

Preferably, the separated zeolitic material is washed until the pH ofthe washing agent, preferably the washwater, is in the range of from 6to 8, preferably from 6.5 to 7.5.

Furthermore, the inventive process can optionally comprise one or moredrying steps. In general, any conceivable means of drying can be used.Drying procedures preferably include heating and/or applying vacuum tothe zeolitic material. In envisaged embodiments of the presentinvention, one or more drying steps may involve spray drying, preferablyspray granulation, of the zeolitic material.

In embodiments which comprise at least one drying step, the dryingtemperatures are preferably in the range of from 25° C. to 150° C., morepreferably of from 60 to 140° C., more preferably of from 70 to 130° C.and even more preferably in the range of from 75 to 125° C. Thedurations of drying are preferably in the range of from 2 to 48 h, morepreferably in the range of 4 to 36 hours, more preferably of from 6 to24 h, and even more preferably of from 8 to 12 h.

In general, the optional washing and/or isolation and/or ion-exchangeprocedures comprised in the inventive process can be conducted in anyconceivable order and repeated as often as desired.

Therefore, according to preferred embodiments of the present invention,the process for the preparation of a zeolitic material further comprisesone or more of the following steps of

-   -   (3) isolating the zeolitic material, preferably by filtration,        and/or    -   (4) washing the zeolitic material, and/or    -   (5) drying and/or calcining the zeolitic material, and/or    -   (6) subjecting the zeolitic material to an ion-exchange        procedure,

wherein the steps (3) and/or (4) and/or (5) and/or (6) can be conductedin any order, and wherein one or more of said steps is preferablyrepeated one or more times.

With respect to the calcination of the zeolitic material according to(5) after optional isolation, washing and/or drying thereof, noparticular restriction applies such that in principle said calcinationmay be conducted at any suitable temperature and for any suitableduration. Thus, by way of example, the calcination may be conducted at atemperature in the range of from 400 to 850° C., wherein preferably, thecalcination is conducted at a temperature ranging from 450 to 700° C.,more preferably from 500 to 600° C., and more preferably from 525 to575° C. Furthermore, the duration of the calcination may range anywherefrom 2 to 48 h, wherein the calcination is preferably conducted for aperiod ranging from 3 to 24 h, more preferably from 4 to 12 h, morepreferably from 4.5 to 8 h, and more preferably from 5 to 6 h. Accordingto the inventive process it is particularly preferred that calcinationof the zeolitic material according to (5) is conducted at a temperaturein the range of from 400 to 850° C. for 2 to 48 h, more preferably at atemperature in the range of from 450 to 700° C. for 3 to 24 h, morepreferably at a temperature in the range of from 500 to 600° C. or 4 to12 h, more preferably at a temperature in the range of from 525 to 575°C. for 4.5 to 8 h, and more preferably at a temperature in the range offrom 525 to 575° C. for 5 to 6 h.

Thus, according to the inventive process, the zeolitic materialcrystallized in step (2) can optionally be subject to at least one stepof an ion-exchange procedure, wherein the term “ion-exchange” accordingto the present invention generally refers to non-framework ionicelements and/or molecules contained in the zeolitic material which areaccordingly exchanged by other ions, which are generally provided froman external source. Preferably, the non-framework ionic elementcomprises one or more of the one or more alkali metals M preferablycomprised in the zeolitic material having a CHA-type framework structurecrystallized in step (2), more preferably Na and/or K, and even morepreferably Na.

In general, any conceivable ion-exchange procedure with all possibleionic elements and/or molecules can be conducted on the zeoliticmaterial. Preferably, as ionic elements at least one cation and/orcationic element is employed which is preferably selected from the groupconsisting of H⁺, NH₄ ⁺, Sr, Zr, Cr, Mg, Mo, Fe, Co, Ni, Cu, Zn, Ru, Rh,Pd, Ag, Os, Ir, Pt, Au, and mixtures of two or more thereof, morepreferably from the group consisting of H⁺, NH₄ ⁺, Sr, Cr, Mo, Fe, Co,Ni, Cu, Zn, Ag, and mixtures of two or more thereof, more preferablyfrom the group consisting of H⁺, NH₄ ⁺, Cr, Mg, Mo, Fe, Ni, Cu, Zn, Ag,and mixtures of two or more thereof. According to particularly preferredembodiments of the present invention, the one or more cations and/orcationic elements are selected from the group consisting of Mg, Mo, Fe,Ni, Cu, Zn, Ag, and mixtures of two or more thereof, wherein morepreferably the one or more cation and/or cationic elements comprise Cuand/or Fe, preferably Cu, wherein even more preferably the one or morecation and/or cationic elements consist of Cu and/or Fe, preferably ofCu. Preferably, the zeolitic material is first ion-exchanged with H⁺and/or NH₄ ⁺, and more preferably with NH₄ ⁺, before being subject to afurther ion-exchange procedure, more preferably before being subject toion-exchange with at least one cation and/or cationic element selectedfrom the group consisting of Sr, Zr, Cr, Mg, Mo, Fe, Co, Ni, Cu, Zn, Ru,Rh, Pd, Ag, Os, Ir, Pt, Au, and mixtures of two or more thereof, morepreferably from the group consisting of Sr, Cr, Mo, Fe, Co, Ni, Cu, Zn,Ag, and mixtures of two or more thereof, more preferably from the groupconsisting of Cr, Mg, Mo, Fe, Ni, Cu, Zn, Ag, and mixtures of two ormore thereof, more preferably from the group consisting of Mg, Mo, Fe,Ni, Cu, Zn, Ag, and mixtures of two or more thereof, wherein morepreferably the zeolitic material is first ion-exchanged with one or morecation and/or cationic elements comprising Cu and/or Fe, preferably Cu,wherein more preferably the one or more cation and/or cationic elementsconsist of Cu and/or Fe, preferably of Cu. As regards preferredembodiments of the present invention wherein the zeolitic material isfirst ion-exchanged with an NH₄ ⁺ before being subject to a furtherion-exchange procedure, this may also be achieved by transformation ofH⁺ ions already contained in the zeolitic material into NH₄ ⁺ ions byappropriate treatment with ammonia or any precursor compound thereof. Asregards the one or more ionic non-framework elements which areion-exchanged, there is no particular restriction according to thepresent invention as to which ionic non-framework elements present inthe zeolitic material may be ion-exchanged according to theaforementioned preferred embodiments, wherein preferably the one or moreionic non-framework elements to be exchanged comprise H⁺ and/or analkali metal, the alkali metal preferably being selected from the groupconsisting of Li, Na, K, Cs, and combinations of two or more thereof,more preferably from the group consisting of Li, Na, K, and combinationsof two or more thereof, wherein more preferably the alkali metal is Naand/or K, and even more preferably Na.

According to a further embodiment of the inventive process, the zeoliticmaterial crystallized in step (2) is directly subject to at least onestep of drying, preferably to spray drying and or spray granulation,without isolating, washing, or drying of the zeolitic materialbeforehand. Directly subjecting the mixture obtained from step (2) ofthe inventive process to a spray drying or spray granulation stage hasthe advantage that isolation and drying is performed in a single stage.Consequently, according to this embodiment of the present invention, aneven more preferred process is provided wherein the number ofpost-synthesis workup steps is minimized, as a result of which thezeolitic material can be obtained from a highly simplified process.

According to a further embodiment of the present invention, the zeoliticmaterial obtained from crystallization in step (2) is subject to atleast one isolating step prior to being subject to at least oneion-exchange procedure, preferably to at least one isolating stepfollowed by at least one washing step, and more preferably to at leastone isolating step followed by at least one washing step followed by atleast one drying step.

In general, the zeolitic material obtained according to the inventiveprocess may be any conceivable zeolitic material, wherein preferablysaid zeolitic material formed in step (2) comprises one or more zeoliteshaving the CHA-type framework structure. Among the preferred zeoliticmaterials comprising one or more zeolites having the CHA-type frameworkstructure, there is no particular restriction neither with respect tothe type and/or number thereof, nor with respect to the amount thereofin the zeolitic material. According to preferred embodiments of thepresent invention, the one or more zeolites having the CHA frameworkstructure comprise one or more zeolites selected from the groupconsisting of (Ni(deta)₂)-UT-6, Chabazite, |Li—Na|[Al—Si—O]-CHA, DAF-5,Dehyd. Na-Chabazite, K-Chabazite, LZ-218, Linde D, Linde R, Phi, SSZ-62,UiO-21, Willhendersonite, ZK-14, ZYT-6, and mixtures of two or morethereof, more preferably from the group consisting of (Ni(deta)₂)-UT-6,Chabazite, |Li—Na|[Al—Si—O]-CHA, DAF-5, Dehyd. Na-Chabazite, K-Chabazite(Iran), LZ-218, Linde D, Linde R, Phi, SSZ-62, UiO-21, Willhendersonite,ZK-14, ZYT-6, and combinations of two or more thereof, wherein even morepreferably the zeolitic material formed in step (2) comprises Chabazite.

According to the inventive process, it is particularly preferred thatthe mixture provided in step (1) and crystallized in step (2) at nopoint contains any substantial amount of an organic structure directingagent other than the one or more tetraalkylammonium cationR⁵R⁶R⁷R⁸N⁺-containing compounds according to any of the particular andpreferred embodiments of the present invention, wherein such organicstructure directing agents other than the tetraalkylammonium compoundsused in the inventive process preferably designate any other conceivableorganotemplates which may suitably be used in the synthesis of zeoliticmaterials having a CHA-type framework structure either by themselves, orin combination with the one or more tetraalkylammonium cationR⁵R⁶R⁷R⁸N⁺-containing compounds according to the present invention.According to a preferred meaning of the present invention, the organicstructure directing agent other than the one or more tetraalkylammoniumcation R⁵R⁶R⁷R⁸N⁺-containing compounds designates any one or morecompounds selected from dialkyl amines, and/or heterocyclic amines,including any combination of two or more thereof, wherein preferablysaid one or more other organic structure directing agent is selectedfrom the group consisting of di(C₁-C₅)alkyl amines, oxygen containingheteroxyclic amines with 5 to 8 ring members, and combinations of two ormore thereof, more preferably from the group consisting ofdi(C₂-C₄)alkyl amines, oxygen containing heteroxyclic amines with 5 to 7ring members, and combinations of two or more thereof, more preferablyfrom the group consisting of di(C₂-C₃)alkyl amines, oxygen containingheteroxyclic amines with 5 or 6 ring members, and combinations of two ormore thereof, and/or related organotemplates such as any suitableN-alkyl-3-quinuclidinol compound, N,N,N-trialkyl-exoaminonorbornanecompound, N,N,N-trimethyl-1-adamantylammonium compound,N,N,N-trimethyl-2-adamantylammonium compound,N,N,N-trimethylcyclohexylammonium compound,N,N-dimethyl-3,3-dimethylpiperidinium compound,N,N-methylethyl-3,3-dimethylpiperidinium compound,N,N-dimethyl-2-methylpiperidinium compound,1,3,3,6,6-pentamethyl-6-azonio-bicyclo(3.2.1)octane compound,N,N-dimethylcyclohexylamine compound, or any suitableN,N,N-trimethylbenzylammonium compound, including combinations of two ormore thereof. According to particularly preferred embodiments of thepresent invention, the mixture provided in step (1) does not contain anysubstantial amount of a trimethyl benzyl ammonium containing compound,and preferably not any substantial amount of a trialkyl benzyl ammoniumcompound, wherein even more preferably the mixture provided in step (1)only contains one or more N,N,N-trimethyl-cyclohexylammonium compoundsand preferably N,N,N-trimethyl-cyclohexylammonium hydroxide as structuredirecting agent for the crystallization of a zeolitic material having aCHA-type framework structure in step (2).

Therefore, it is preferred according to the present invention that themixture provided in step (1) does not contain any substantial amount ofa trimethyl benzyl ammonium containing compound, preferably of atrialkyl benzyl ammonium compound wherein preferably the mixtureprovided in step (1) does not contain any substantial amount of anorganotemplate other than the one or more tetraalkylammonium cationR⁵R⁶R⁷R⁸N⁺-containing compounds as structure directing agent, whereinmore preferably the mixture provided in step (1) does not contain anysubstantial amount of a structure directing agent other than the one ormore tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing compounds, andwherein even more preferably, the mixture provided in step (1) onlycontains one or more N,N,N-trimethyl-cyclohexylammonium compounds andpreferably N,N,N-trimethyl-cyclohexylammonium hydroxide as structuredirecting agent for the crystallization of a zeolitic material having aCHA-type framework structure in step (2).

According to specific embodiments of the present invention, not morethan an impurity of said one or more other organic structure directingagent may, however, be present in the reaction mixture, for example, asa result of said one or more other organic structure directing agentsstill being present in seed crystals preferably used in the inventiveprocess. Such other organotemplates contained in seed crystal materialmay not, however, participate in the crystallization process since theyare trapped within the seed crystal framework and therefore may not actstructure directing agents within the meaning of the present invention.

Within the meaning of the present invention, the term “substantially” asemployed in the present application with respect to the amount of anyone or more organotemplate other than the one or more tetraalkylammoniumcation R⁵R⁶R⁷R⁸N⁺-containing compounds as structure directing agentcontained in the mixture provided in step (1) indicates an amount of 0.1wt.-% or less of the total amount of any other one or moreorganotemplate, preferably 0.05 wt.-% or less, more preferably 0.001wt.-% or less, more preferably 0.0005 wt.-% or less, and even morepreferably 0.0001 wt.-% or less thereof. Said amounts of one or moreother organotemplates, if at all present an any one of the materialsused in the synthetic process, may also be denoted as “impurities” or“trace amounts” within the meaning of the present invention.Furthermore, it is noted that the terms “organotemplate” and “organicstructure directing agent” are synonymously used in the presentapplication.

According to the process of the present invention, seed crystals mayoptionally be provided in step (1), wherein said seed crystalspreferably comprise a zeolitic material of the same type of frameworkstructure as obtained from crystallization in step (2), wherein morepreferably the seed crystals comprise a zeolitic material as obtainedaccording to the inventive process. According to particularly preferredembodiments, the seed crystals comprise one or more zeolitic materialshaving a CHA-type framework structure. According to said preferredembodiments, the seed crystals may comprise any zeolitic material havinga CHA-type framework structure, provided that a zeolitic material iscrystallized in step (2), which is preferably a zeolitic material havingthe CHA-type framework structure, wherein more preferably the zeoliticmaterial having a CHA-type framework structure comprised in the seedcrystals is a zeolitic material obtained according to the inventiveprocess, and wherein even more preferably the zeolitic material having aCHA-type framework structure comprised in the seed crystals is the sameas the zeolitic material having a CHA-type framework structure which isthen crystallized in step (2). Particularly preferred according to thepresent invention are seed crystals comprising one or more zeolitesselected from the group consisting of (Ni(deta)₂)-UT-6, Chabazite,|Li—Na|[Al—Si—O]-CHA, DAF-5, Dehyd, Na-Chabazite, K-Chabazite, LZ-218,Linde D, Linde R, Phi, SSZ-62, UiO-21, Willhendersonite, ZK-14, ZYT-6,and mixtures of two or more thereof, wherein more preferably the seedcrystals comprise one or more zeolites selected from the groupconsisting of(Ni(deta)₂)-UT-6, Chabazite, |Li—Na|[Al—Si—O]-CHA, DAF-5,Dehyd. Na-Chabazite, K-Chabazite (Iran), LZ-218, Linde D, Linde R, Phi,SSZ-62, Willhendersonite, ZK-14, ZYT-6, and mixtures of two or morethereof, and wherein even more preferably the seed crystals compriseChabazite. According to an even more preferred embodiments Chabazite isemployed as seed crystals in the inventive process, wherein preferablysaid Chabazite seed crystals are either obtainable according to theinventive process or have been obtained according to said process.

Concerning the Chabazite seed crystals preferably provided in step (1),there is in principle no particular restriction as the their chemicaland/or physical properties, provided that a zeolitic material having aCHA-type framework structure comprising YO₂ and X₂O₃ is crystallized instep (2). Thus, as regards the SiO₂:Al₂O₃ molar ratio of the Chabaziteseed crystals preferably used in the inventive process, no particularrestriction applies, such that the seed crystals may display anysuitable SiO₂:Al₂O₃ molar ratio. Thus, by way of examples, theSiO₂:Al₂O₃ molar ratio of the preferred Chabazite seed crystals mayrange anywhere from 4 to 200, preferably from 10 to 100, more preferablyfrom 16 to 60, more preferably from 20 to 40, more preferably from 25 to35, and even more preferably from 29 to 33.

Furthermore, regarding the non-framework ionic elements and/or moleculeswhich may be contained in the Chabazite seed crystals preferablyprovided in step (1) of the inventive process, again no particularrestrictions apply, wherein preferably the one or more non-frameworkelements and/or molecules comprise at least one cation and/or cationicelements, wherein said at least one cation and/or cationic element ispreferably selected from the group consisting of H⁺, NH₄ ⁺, Li, Na, K,Cs, and combinations of two or more thereof, more preferably from thegroup consisting of H⁺, NH₄ ⁺, Na, K, and combinations of two or morethereof, more preferably from the group consisting of H⁺, NH₄ ⁺, Na, andcombinations of two or more thereof, wherein more preferably the atleast one cation and/or cationic element is H⁺ and/or Na, morepreferably Na.

As regards the porosity and/or surface area of the Chabazite seedcrystals preferably provided in step (1) of the inventive process, thesemay adopt any suitable values. Thus, as regards the BET surface area ofthe preferred Chabazite seed crystals as determined according to DIN66135, it may accordingly range anywhere from 100 to 850 m²/g, whereinpreferably the surface area is comprised in the range of from 300 to 800m²/g, more preferably from 400 to 750 m²/g, more preferably from 500 to700 m²/g, more preferably from 550 to 650 m²/g, and even more preferablyfrom 580 to 640 m²/g. According to particularly preferred embodiments ofthe present invention, the BET surface area of the Chabazite seedcrystals preferably provided in step (1) of the inventive process asdetermined according to DIN 66135 ranges from 600 to 630 m²/g.

Concerning the average particle size of the Chabazite seed crystalspreferably provided in step (1) of the inventive process, they mayaccordingly display any conceivable particle size, and in particular anyconceivable particle size D10 and/or D50 and/or D90. Thus, as concernsthe particle size D10 of the preferred Chabazite seed crystals, noparticular restriction applies such that by way of example, the particlesize D10 thereof may be comprised in the range of anywhere from 5 to 200nm. According to the present invention it is however preferred that theparticle size D10 of the preferred Chabazite seed crystals lies withinthe range of from 10 to 150 nm, more preferably from 15 to 100 nm, morepreferably from 20 to 70 nm, and more preferably from 25 to 50 nm.According to the present invention it is particularly preferred that theparticle size D10 of the preferred Chabazite seed crystals lies withinthe range of from 30 to 40 nm.

With respect to the average particle size D50 of the preferred Chabaziteseed crystals, same applies accordingly such that in principle saidvalues may adopt any conceivable value. Thus, by way of example, theaverage particle size D50 of the preferred Chabazite seed crystals maybe comprised in the range of from 50 to 1,000 nm, wherein preferably theaverage particle size D50 lies in the range of from 100 to 700 nm, morepreferably from 150 to 500 nm, more preferably from 200 to 400 nm, andmore preferably from 250 to 350 nm. According to the present inventionit is particularly preferred that the average particle size D50 of thepreferred Chabazite seed crystals lies in the range of from 270 to 290nm.

As mentioned in the foregoing relative to the particle sizes D10 andD50, in general, no particular restrictions apply relative to theparticle size D90 as well such that the the preferred Chabazite seedcrystals may adopt any conceivable particle size D90 value. Thus, by wayof example, the particle size D90 of the preferred Chabazite seedcrystals may be comprised in the range of anywhere from 500 to 3,000 nm,wherein it is preferable that the particle size D90 is comprised in therange of from 800 to 2,500 nm, more preferably from 1,000 to 2,000 nm,more preferably from 1,200 to 1,800 nm, more preferably from 1,300 to1,700 nm, more preferably from 1,400 to 1,650 nm, more preferably from1,450 to 1,600 nm, and more preferably from 1,500 to 1,580 nm. Accordingto the present invention it is particularly preferred that the particlesize D90 of the preferred Chabazite seed crystals is comprised in therange of from 1,530 to 1,550 nm.

Finally, the Chabazite seed crystals preferably provided in step (1) maybe subject to any suitable treatment prior to their use. Thus, by way ofExample, the preferred Chabazite seed crystals may be subject to anyion-exchange and/or thermal treatment prior to their use, such that theChabazite seed crystals may be used as such, and in particular in theuncalcined form as obtained from synthesis, or may be subject tocalcination prior to their use. According to the inventive process it ishowever preferred that the preferred Chabazite seed crystals arecalcined prior to their use in the inventive process, whereincalcination is preferably performed at a temperature ranging from 400 to850° C., wherein preferably, the calcination is conducted at atemperature ranging from 450 to 700° C., more preferably from 525 to650° C., and more preferably from 575 to 625° C. Furthermore, theduration of the calcination may range anywhere from 1 to 48 h, whereinthe calcination is preferably conducted for a period ranging from 2 to24 h, more preferably from 3 to 12 h, more preferably from 3.5 to 8 h,and more preferably from 4 to 6 h.

According to the inventive process, any suitable amount of seed crystalscan be provided in the mixture according to step (1), provided that azeolitic material is crystallized in step (2). In general, the amount ofseed crystals contained in the mixture according to step (1) ranges from0.1 to 20 wt.-% based on 100 wt.-% of YO₂ in the at least one source forYO₂, preferably from 0.5 to 15 wt.-%, more preferably from 1 to 12wt.-%, more preferably from 1.5 to 10 wt.-%, more preferably from 2 to 8wt.-%, more preferably from 2.5 to 6 wt.-%, and more preferably from 3to 5 wt.-%. According to particularly preferred embodiments of theinventive process, from 3.5 to 4.5 wt.-% of seed crystals according toany of the particular and preferred embodiments of the present inventionare employed, based on 100 wt-% of YO₂ in the at least one source forYO₂ provided in step (1) of the inventive process.

Concerning the further elements or compounds which may be contained inthe mixture provided in step (1), there is no particular restrictionaccording to the present invention in this respect, provided that azeolitic material having the CHA-type framework structure may beobtained in step (2) of the inventive process. Thus, according toparticular embodiments of the present invention, the mixture provided instep (1) may comprise one or more alkali metals M, wherein within themeaning of the present invention, the one or more alkali metals Mpreferably stands one or more elements selected from the groupconsisting of Li, Na, K, Rb, Cs, and combinations of two or morethereof, more preferably from the group consisting of Li, Na, K, andcombinations of two or more thereof, wherein even more preferably theone of more alkali metals M stand for Na and/or K, and even morepreferably for Na.

As regards particular embodiments of the present invention wherein themixture provide in step (1) comprises one or more alkali metals Maccording to any of the particular and preferred meanings of the presentinvention, there is no particular restriction as to the amounts in whichthey may be contained in said mixture, provided that a zeolitic materialhaving the CHA-type framework structure may be obtained in step (2) ofthe inventive process. According to particularly preferred embodimentsof the present invention, however, the mixture provided in step (1)which is crystallized in step (2) contains 3 wt.-% or less of one ormore alkali metals M based on 100 wt-% of YO₂. According to embodimentswhich are further preferred, the mixture provided in step (1) contains 1wt.-% or less of one or more alkali metals M, more preferably 0.5 wt.-%or less, more preferably 0.1 wt.-% or less, more preferably 0.05 wt.-%or less, more preferably 0.01 wt.-% or less, more preferably 0.005 wt.-%or less, more preferably 0.001 wt.-% or less, more preferably 0.0005wt.-% or less, and even more preferably 0.0001 wt.-% or less of one ormore metals M based on 100 wt.-% of YO₂. According to particularlypreferred embodiments of the present invention it is even furtherpreferred that the mixture provided in step (1) and crystallized in step(2) contains no alkali metal M.

The present invention further comprises preferred embodiments of theinventive process wherein one or more sources of one or more elementssuitable for isomorphous substitution of at least a portion of the Yatoms and/or of the X atoms in the zeolite framework structure havingthe CHA-type framework structure is added to the mixture according tostep (1). In this respect, there is no particular restriction accordingto the present invention neither as to the type and/or number nor as tothe amount of which said one or more sources of one or more elementssuitable for isomorphous substitution may be employed. Thus, inprinciple, any one or more elements suitable for isomorphoussubstitution may be employed provided that they are at least partlyincorporated into the framework structure of the zeolitic materialcrystallized in step (2) of the inventive process. According topreferred embodiments, the one or more elements are selected from thegroup consisting of B, Fe, Ti, Sn, Ga, Ge, Zr, V, Nb, Cu, Zn, Li, Be,and mixtures of two or more thereof, wherein more preferably the one ormore elements are selected from the group consisting of B, Fe, Ti, Sn,Zr, Cu, and mixtures of two or more thereof. According to particularlypreferred embodiments of the present invention, the one or more elementssuitable for isomorphous substitution provided in step (1) comprise Feand/or Cu, preferably Fe, wherein even more preferably the one or moreelements are Fe and/or Cu. According to embodiments of the presentinvention which are particularly preferred, Cu is added as the elementsuitable for isomorphous substitution of at least a portion of the Yand/or of the X atoms in the mixture according to step (1).

As noted above, no particular restriction applies with respect to theamount of the one or more sources for isomorphous substitutionpreferably provided in the mixture in step (1) of the inventive process.Thus, by way of example, the molar ratio of YO₂ to the one or moreelements suitable for isomorphous substitution in the mixture of step(1) of the inventive process may be comprised in the range of anywherefrom 5 to 200, wherein it is preferred that said ratio is comprised inthe range of from 10 to 100, more preferably of from 20 to 70, and evenpreferably of from 25 to 50. According to particularly preferredembodiments of the present invention wherein one or more elementssuitable for isomorphous substitution are included in the mixture ofstep (1), it is preferred that the molar ratio of YO₂ to said one ormore elements is comprised in the range of from 30 to 40.

The present invention further relates to a zeolitic material having aCHA-type framework structure which is either obtained by the processaccording to the present invention or by any conceivable process whichleads to a zeolitic material having a CHA-type framework structure asobtainable according to the inventive process, wherein in particular theinventive process designates any of the particular and preferredembodiments thereof as defined in the present application.

Furthermore, the present invention also relates to a synthetic zeoliticmaterial having a CHA-type framework structure, preferably obtainableand/or obtained according to the process of any of claims 1 to 24,wherein the CHA-type framework structure comprises YO₂ and X₂O₃, whereinY is a tetravalent element and X is a trivalent element, and wherein thethe IR-spectrum of the zeolitic material comprises:

-   -   a first absorption band (B1) in the range of from 3,720 to 3,740        cm⁻¹; and    -   a second absorption band (B2) in the range of from 1,850 to        1,890 cm⁻¹;

wherein the ratio of the maximum absorbance of the first absorption bandto the second absorption band B1:B2 is comprised in the range of from0.5 to 1.55, preferably from 0.8 to 1.45, more preferably from 1.0 to1.4, more preferably from 1.1 to 1.38, more preferably from 1.2 to 1.37,more preferably from 1.3 to 1.36, and more preferably from 1.33 to 1.35.

With respect to the first absorption band (B1) in the range of from3,720 to 3,740 cm⁻¹, said band is attributed to stretching vibration ofhydroxyl groups from isolated or nearly isolated silanol in the zeoliticmaterial, and in particular from surface silanol groups. According tothe present invention, it is preferred that the first absorption band(B1) is in the range of from 3,722 to 3,738 cm⁻¹, more preferably from3,724 to 3,736 cm⁻¹, more preferably from 3,726 to 3,734 cm⁻¹, morepreferably from 3,728 to 3,733 cm⁻¹, and more preferably from 3,729 to3,732 cm⁻¹. As concerns the second absorption band (B2) in the range offrom 1,850 to 1,890 cm⁻¹ on the other hand, it is preferred that saidabsorption is in the range of from 1,855 to 1,885 cm⁻¹, more preferablyfrom 1,860 to 1,880 cm⁻¹, more preferably from 1,865 to 1,875 cm⁻¹, andmore preferably from 1,870 to 1,872 cm⁻¹. Thus, according to the presentinvention it is particularly preferred that the first absorption band(B1) is in the range of from 3,722 to 3,740 cm⁻¹ and the secondabsorption band (B2) is in the range of from 1,855 to 1,885 cm⁻¹, morepreferably that (B1) is in the range of from 3,724 to 3,740 cm⁻¹ and(B2) is in the range of from 1,860 to 1,880 cm⁻¹, more preferably that(B1) is in the range of from 3,726 to 3,740 cm⁻¹ and (B2) is in therange of from 1,865 to 1,875 cm⁻¹, more preferably that (B1) is in therange of from 3,728 to 3,740 cm⁻land (B2) is in the range of from 1,870to 1,872 cm⁻¹, and more preferably that (B1) is in the range of from3,729 to 3,740 cm⁻¹ and (B2) is in the range of from 1,870 to 1,872cm⁻¹.

As regards the state of the synthetic zeolitic material having aCHA-type framework structure from which the IR-spectrum is obtained, ingeneral, no particular restriction applies for the synthetic zeoliticmaterials of the present invention such that the values of theabsorption bands and the ratio of the maximum absorbance if the firstand second absorbtion bands in the IR-spectrum as defined in the presentapplication may refer to the IR-spectrum of the synthetic zeoliticmaterial as obtained directly after crystallization or after anysuitable workup thereof by any one or more suitable washing, drying, andcalcination steps. According to the present invention it is howeverpreferred that the IR-spectrum is directly obtained from the zeoliticmaterial as-crystallized wherein after isolation, washing and dryingthereof, the material has only been subject to calcination for removalof the organic template, wherein preferably calcination has beenconducted according to any of the particular and preferred embodimentsas defined in the present application, wherein more preferablycalcination has been conducted at 550° C. for a duration of 5 h underair.

Regarding the further physical and/or chemical characteristics of thesynthetic zeolitic material according to the present invention, noparticular restrictions apply, provided that the zeolitic materialdisplays a CHA-type framework structure and that the IR-spectrum of thesynthetic zeolitic material displays absorption bands according to anyof the particular and preferred embodiments of the present invention asdefined in the present application. Consequently, as regards the averageparticle size of the zeolitic material, it may accordingly display anyconceivable particle size, and in particular any conceivable particlesize D10 and/or D50 and/or D90. Within the meaning of the presentinvention, the terms “D10”, “D50”, and “D90” respectively refer to theparticle size in number of the synthetic zeolitic material of thepresent invention, wherein D10 refers to the particle size wherein 10%of the particles of the zeolitic material by number lie below saidvalue, D50 refers to the particle size wherein 50% of the particles ofthe zeolitic material by number lie below said value, and D90accordingly refers to the particle size wherein 90% of the particles ofthe zeolitic material by number lie below said particle size.

As concerns the particle size D10 of the inventive zeolitic material, noparticular restriction applies such that by way of example, the particlesize D10 of the zeolitic material may be comprised in the range ofanywhere from 500 to 2,500 nm. According to the present invention it ishowever preferred that the particle size D10 of the zeolitic materiallies within the range of from 600 to 2,000 nm, more preferably from 800to 1,800 nm, more preferably from 1,000 to 1,600 nm, and more preferablyfrom 1,200 to 1,500 nm. According to the present invention it isparticularly preferred that the particle size 010 of the zeoliticmaterial lies within the range of from 1,300 to 1,400 nm.

According to the present invention, it is alternatively preferred thatthe particle size D10 of the zeolitic material lies within the range offrom 200 to 1,000 nm, more preferably from 250 to 800 nm, morepreferably from 300 to 600 nm, and more preferably from 325 to 500 nm.According to the present invention it is particularly preferred that theparticle size D10 of the zeolitic material lies within the range of from350 to 450 nm.

With respect to the average particle size D50 of the inventive zeoliticmaterial, same applies accordingly such that in principle said valuesmay adopt any conceivable value. Thus, by way of example, the averageparticle size D50 of the zeolitic material may be comprised in the rangeof from 700 to 3,500 nm, wherein preferably the average particle sizeD50 lies in the range of from 900 to 3,000 nm, more preferably from1,100 to 2,800 nm, more preferably from 1,300 to 2,500 nm, morepreferably from 1,500 to 2,200 nm, more preferably from 1,550 to 2,000nm, and more preferably from 1,600 to 1,900 nm. According to the presentinvention it is particularly preferred that the average particle sizeD50 of the inventive zeolitic material lies in the range of from 1,650to 1,850 nm.

According to the present invention, it is alternatively preferred thatthe particle size D50 of the zeolitic material lies within the range offrom 400 to 1,400 nm, more preferably from 450 to 1,100 nm, morepreferably from 500 to 900 nm, and more preferably from 525 to 700 nm.According to the present invention it is particularly preferred that theparticle size D50 of the zeolitic material lies within the range of from550 to 650 nm.

As mentioned in the foregoing relative to the particle sizes D10 andD50, in general, no particular restrictions apply relative to theparticle size D90 as well such that the inventive zeolitic material mayadopt any conceivable particle size D90 value. Thus, by way of example,the particle size D90 of the inventive zeolitic material may becomprised in the range of anywhere from 900 to 4,500 nm, wherein it ispreferable that the particle size D90 is comprised in the range of from1,100 to 4,000 nm, more preferably from 1,400 to 3,800 nm, morepreferably from 1,600 to 3,500 nm, more preferably from 1,800 to 3,200nm, more preferably from 2,000 to 2,900 nm, more preferably from 2,100to 2,700 nm, more preferably from 2,200 to 2,600 nm, and more preferablyfrom 2,250 to 2,550 nm. According to the present invention it isparticularly preferred that the particle size D90 of the zeoliticmaterial is comprised in the range of from 2,300 to 2,500 nm.

According to the present invention, it is alternatively preferred thatthe particle size D90 of the zeolitic material lies within the range offrom 800 to 2,000 nm, more preferably from 1,000 to 1,700 nm, morepreferably from 1,100 to 1,500 nm, and more preferably from 1,150 to1,300 nm. According to the present invention it is particularlypreferred that the particle size D90 of the zeolitic material lieswithin the range of from 1,200 to 1,250 nm.

As for the determination of the IR-spectra of the inventive zeoliticmaterials, in principle no particular restrictions apply as to the stateof the zeolitic material in which the particle size D10 and/or D50and/or D90 is determined. Thus, within the meaning of the presentinvention, the particle size D10 and/or D50 and/or D90 of the inventivezeolitic material refers to the respective particle size of the zeoliticmaterial either in the as-crystallized state or after having beensubject to any suitable workup thereof by any one or more suitablewashing, drying, and calcination steps. According to the presentinvention it is however preferred that the particle size D10 and/or D50and/or D90 is directly obtained from the zeolitic materialas-crystallized wherein preferably the zeolitic material has not beensubject to any further treatment after crystallization other thanoptional isolation, optional washing, and/or optional drying. Thus,according to the present invention it is yet further preferred that theparticle size D10 and/or D50 and/or D90 as defined in the presentapplication are directly obtained from the as-crystallized zeoliticmaterial after isolation, washing, and/or drying thereof, and preferablyafter isolation, washing, and drying thereof. It is, however, furtherpreferred according to the present invention that the particle size D10and/or D50 and/or D90 is directly obtained from the zeolitic materialas-crystallized wherein after isolation, washing and drying thereof, thematerial has only been subject to calcination for removal of the organictemplate, wherein preferably calcination has been conducted according toany of the particular and preferred embodiments as defined in thepresent application, wherein more preferably calcination has beenconducted at 550° C. for a duration of 5 h under air.

According to the present invention it is further preferred that theparticle size D10, the average particle size D50, and the particle sizeD90 of the zeolitic material is comprised within defined ranges whereinthe particle size D10 of the zeolitic material is comprised in the rangeof from 1,200 to 1,500 nm, more preferably from 1,250 to 1,450 nm, andmore preferably from 1,300 to 1,400 nm, and the average particle size050 of the zeolitic material is comprised in the range of from 1,550 to1,950 nm, preferably from 1,600 to 1,900 nm, and more preferably from1,650 to 1,850 nm, and the particle size D90 of the zeolitic material iscomprised in the range of from 2,000 to 2,900 nm, preferably from 2,100to 2,700 nm, more preferably from 2,200 to 2,600 nm, more preferablyfrom 2,250 to 2,550 nm, and more preferably from 2,300 to 2,500 nm. Morepreferably, it is preferred that the particle size D10 of the zeoliticmaterial is comprised in the range of from 1,200 to 1,500 nm, theaverage particle size D50 of the zeolitic material is comprised in therange of from 1,550 to 1,950 nm, and the particle size D90 of thezeolitic material is comprised in the range of from 2,000 to 2,900 nm,preferably from 2,100 to 2,700 nm. More preferably, the particle sizeD10 of the zeolitic material is comprised in the range of from 1,250 to1,450 nm, the average particle size D50 is comprised in the range offrom 1,600 to 1,900 nm and the particle size D90 is comprised in therange of from 2,200 to 2,600 nm, more preferably from 2,250 to 2,550 nm.According to the present invention it is particularly preferred that theparticle size D10 of the zeolitic material is comprised in the range offrom 1,300 to 1,400 nm, the average particle size D50 in the range offrom 1,650 to 1,850 nm, and the particle size D90 is comprised in therange of from 2,300 to 2,500 nm.

According to the present invention it is alternatively preferred thatthe particle size 010, the average particle size D50, and the particlesize D90 of the zeolitic material is comprised within defined rangeswherein the particle size D10 of the zeolitic material is comprised inthe range of from 325 to 500 nm, and the average particle size D50 ofthe zeolitic material is comprised in the range of from 525 to 700 nm,and the particle size 090 of the zeolitic material is comprised in therange of from 800 to 2,000 nm. More preferably, it is preferred that theparticle size D10 of the zeolitic material is comprised in the range offrom 350 to 450 nm, the average particle size D50 of the zeoliticmaterial is comprised in the range of from 550 to 650 nm, and theparticle size D90 of the zeolitic material is comprised in the range offrom 1,100 to 1,500 nm.

According to the present invention, it is preferred that at least aportion of the Y atoms and/or of the X atoms of the CHA-type frameworkstructure of the zeolitic materials is isomorphously substituted by oneor more elements. In this respect, there is no particular restriction asto the one or more elements which may substitute Y atoms and/or X atomsof the CHA-type framework structure wherein preferably said elements areselected from the group consisting of B, Fe, Ti, Sn, Ga, Ge, Zr, V, Nb,Cu, Zn, Li, Be, and mixtures of two or more thereof, wherein even morepreferably, the one or more elements are selected from the groupconsisting of B, Fe, Ti, Sn, Zr, Cu, and mixtures of two or morethereof. According to particularly preferred embodiments and inparticular according to particularly preferred embodiments of thealternative zeolitic material of the present invention, at least aportion of the Y atoms and/or of the X atoms in the CHA-type frameworkstructure is isomorphously substituted by Fe and/or Cu, and preferablyby Cu.

As regards the amount of the one or more elements in the zeoliticmaterials which substitute at least a portion of the Y atoms and/or ofthe X atoms in the CHA-type framework structure, no particularrestriction applies according to the present invention. Thus, by way ofexample, the molar ratio of YO₂ to the one or more elementsisomorphously substituted in the CHA-type framework structure may rangeanywhere from 2 to 100, wherein the molar ratio is preferably comprisedin the range of from 5 to 50, more preferably of from 8 to 30, morepreferably of from 10 to 20, and even more preferably of from 13 to 15.According to particularly preferred embodiments, the molar ratio of YO₂to the one or more elements isomorphously substituting Y atoms and/or Xatoms in the CHA-type framework structure are comprised in the range offrom 13 to 15.

As regards the CHA-type framework structure of the inventive zeoliticmaterial, besides YO₂ and X₂O₃ contained therein as framework elements,no particular restriction applies as to any other elements which may becontained therein as further framework elements. Thus, besides or inaddition to the preferred elements suitable for isomorphous substitutionaccording the particular and preferred embodiments of the presentinvention which may be contained in the CHA-type framework structure ofthe zeolitic material, any further one or more elements than theaforementioned may also be contained therein as framework elements inaddition to the one or more tetravalent elements Y and the one or moretrivalent elements X. According to particular embodiments of the presentinvention, however, it is preferred that the zeolitic material having aCHA-type framework does not contain any substantial amount of P and/orAs therein as framework element. Within the meaning of the presentinvention, the term “substantial” with respect to the amount of anelement contained in the framework structure of the inventive zeoliticmaterial preferably indicates an amount of 5 wt.-% or less of aframework element based on 100 wt-% of YO₂ contained in the frameworkstructure, preferably an amount of 1 wt.-% or less, more preferably of0.5 wt.-% or less, more preferably of 0.1 wt.-% or less, more preferablyof 0.05 wt.-% or less, more preferably of 0.01 wt.-% or less, morepreferably of 0.005 wt.-% or less, more preferably of 0.001 wt.-% orless, more preferably of 0.0005 wt.-% or less, and even more preferablyof 0.0001 wt.-% or less of a framework element based on 100 wt.-% ofYO₂.

According to said particularly preferred embodiments wherein zeoliticmaterial having a CHA-type framework does not contain any substantialamount of P and/or As, it is yet further preferred according to thepresent invention that the CHA-type framework does not contain anysubstantial amount of one or more elements selected from the groupconsisting of P, As, V, and combinations of two or more thereof, andmore preferably no substantial amount of any one or more elementsselected from the group consisting of P, As, Sb, Bi, V, Nb, Ta, andcombinations of two or more thereof. According to yet furtherparticularly preferred embodiments of the present invention, theinventive zeolitic material having a CHA-type framework structure doesnot contain any substantial amount of any pentavalent elements Z asframework element.

It is further preferred according to the present invention that thezeolitic material does not comprise any substantial amount of SSZ-13and/or SSZ-15, wherein within the meaning of the present invention“substantial” with respect to the amount of SSZ-13 and/or SSZ-15 refersto an amount of 5 wt.-% or less thereof based on 100 wt-% of thezeolitic material having a CHA-type framework structure according to anyof the particular and preferred embodiments of the present invention,and preferably to an amount of 1 wt.-% or less, more preferably of 0.5wt.-% or less, more preferably of 0.1 wt.-% or less, more preferably of0.05 wt.-% or less, more preferably of 0.01 wt.-% or less, morepreferably of 0.005 wt.-% or less, more preferably of 0.001 wt.-% orless, more preferably of 0.0005 wt.-% or less, and even more preferablyof 0.0001 wt.-% or less of SSZ-13 and/or SSZ-15.

Concerning YO₂:X₂O₃ molar ratio displayed by the zeolitic materials ofthe present invention, any conceivable molar ratio may be adopted. Thus,by way of example, the YO₂:X₂O₃ molar ratio of the inventive materialsmay be comprised anywhere in the range of from 4 to 200, whereinpreferably the YO₂:X₂O₃ molar ratio is comprised in the rage of from 10to 100, more preferably of from 16 to 60, more preferably of from 20 to40, and even more preferably of from 23 to 35. According to particularlypreferred embodiments of the present invention, the YO₂:X₂O₃ molar ratioof the zeolitic materials is comprised in the range of from 25 to 30.

According to the present invention, the zeolitic materials having anCHA-type framework structure comprise YO₂. In principle, Y stands forany conceivable tetravalent element, Y standing for either or severaltetravalent elements. Preferred tetravalent elements according to thepresent invention include Si, Sn, Ti, Zr, and Ge, and combinationsthereof. More preferably, Y stands for Si, Ti, or Zr, or any combinationof said tetravalent elements, even more preferably for Si, and/or Sn.According to the present invention, it is particularly preferred that Ystands for Si.

As regards X₂O₃ optionally comprised in the CHA-framework structure ofthe zeolitic materials, X may in principle stand for any conceivabletrivalent element, wherein X stands for one or several trivalentelements. Preferred trivalent elements according to the presentinvention include Al, B, In, and Ga, and combinations thereof. Morepreferably, X stands for Al, B, or Ga, or any combination of saidtrivalent elements, even more preferably for Al and/or B. According tothe present invention, it is particularly preferred that X stands forAl.

In addition to the framework elements of the zeolitic materials of thepresent invention having an CHA-type framework structure, said zeoliticmaterials preferably further contains one or more types of non-frameworkelements which do not constitute the framework structure and areaccordingly present in the pores and/or cavities formed by the frameworkstructure and typical for zeolitic materials in general. In thisrespect, there is no particular restriction as to the types ofnon-framework elements which may be contained in the zeolitic materials,nor with respect to the amount in which they may be present therein. Itis, however, preferred that the zeolitic materials comprise one or morecation and/or cationic elements as ionic non-framework elements, whereinagain no particular restriction applies as to the type or number ofdifferent types of ionic non-framework elements which may be present inthe zeolitic materials, nor as to their respective amount. According topreferred embodiments of the present invention, the ionic non-frameworkelements preferably comprise one or more cations and/or cationicelements selected from the group consisting of H⁺, NH₄ ⁺, Mg, Sr, Zr,Cr, Mo, Fe, Co, Ni, Cu, Zn, Ru, Rh, Pd, Ag, Os, Ir, Pt, Au, and mixturesof two or more thereof, wherein more preferably these are selected fromthe group consisting of H⁺, NH₄ ⁺, Mg, Sr, Cr, Mo, Fe, Co, Ni, Cu, Zn,Ag, and mixtures of two or more thereof, more preferably from the groupconsisting of H⁺, NH₄ ⁺, Mg, Cr, Mo, Fe, Ni, Cu, Zn, Ag, and mixtures oftwo or more thereof. According to particularly preferred embodiments ofthe present invention, the ionic non-framework elements comprise one ormore cations and/or cationic elements selected from the group consistingof Mg, Mo, Fe, Ni, Cu, Zn, Ag, and mixtures of two or more thereof,wherein more preferably the one or more cation and/or cationic elementscomprise Cu and/or Fe, preferably Cu, wherein even more preferably theone or more cation and/or cationic elements consist of Cu and/or Fe,preferably of Cu.

Concerning the amounts in which the one or more non-framework elementsmay be contained in the inventive zeolitic materials according to any ofthe particular and preferred embodiments of the present invention, nogeneral restriction applies such that in principle any suitable amountof one or more cation and/or cationic elements may be contained asnon-framework element therein. Thus, by way of example, the one or morecation and/or cationic elements comprised as ionic non-frameworkelements in the inventive zeolitic materials may be contained therein inan amount ranging anywhere from 0.01 to 25 wt.-% based on 100 wt.-% ofYO₂ comprised in the zeolitic material, wherein preferably the one ormore cations and/or cationic elements are contained in the zeoliticmaterial in an amount ranging from 0.05 to 15.0 wt.-%, and morepreferably from 0.1 to 10.0 wt.-%, more preferably from 0.5 to 6.0wt.-%, more preferably from 1.0 to 4.0 wt.-%, more preferably from 1.5to 3.5 wt.-%, and more preferably from 2.0 to 3.0 wt.-%. According tothe present invention it is however particularly preferred that the oneor more cations and/or cationic elements are contained in the inventivezeolitic material in an amount ranging from 2.3 to 2.7 wt.-% based on100 wt.-% of YO₂ comprised in the zeolitic material.

As regards the ²⁷Al MAS NMR of the inventive zeolitic materials havingthe CHA-type framework structure comprising X₂O₃ wherein X includes Alor is preferably Al, there is no particular restriction as to the numberand/or respective ppm values and/or relative intensities of the signalswhich may be comprised in the NMR spectrum. According to the presentinvention, however, it is preferred that the ²⁷Al MAS NMR spectrum ofthe inventive materials comprises a first peak (P1) comprised in therange of from 55.0 to 61.5 ppm and a second peak (P2) comprised in therange of from −0.0 to −7.0 ppm, wherein the integration of the first andsecond peaks in the ²⁷Al MAS NMR spectrum of the zeolitic materialpreferably offers a ratio of the integration values P1:P2 of1:(0.005-0.17). More preferably, the first peak (P1) is comprised in therange of from 56.0 to 60.5 ppm, and the second peak (P2) is comprised inthe range of from −0.5 to −6.0 ppm, wherein the integration of the firstand second peaks offers a ratio of the integration values P1:P2 of1:(0.01-0.16). More preferably, the first peak (P1) is comprised in therange of from 56.5 to 60.0 ppm and the second peak (P2) is comprised inthe range of from −1.0 to −5.5 ppm, wherein the integration of the firstand second peaks offers a ratio of the integration values P1:P2 of1:(0.03-0.15). More preferably, the first peak (P1) is comprised in therange of from 57.0 to 59.5 ppm and the second peak (P2) is comprised inthe range of from −1.5 to −5.0 ppm, wherein the integration of the firstand second peaks offers a ratio of the integration values P1:P2 of1:(0.05-0.145). More preferably, the first peak (P1) is comprised in therange of from 57.5 to 59.0 ppm and the second peak (P2) is comprised inthe range of from −2.0 to −4.5 ppm, wherein the integration of the firstand second peaks offers a ratio of the integration values P1:P2 of1:(0.08-0.14). More preferably, the first peak (P1) is comprised in therange of from 57.8 to 58.7 ppm and the second peak (P2) is comprised inthe range of from −2.3 to −4.1 ppm, wherein the integration of the firstand second peaks offers a ratio of the integration values P1:P2 of1:(0.10-0.135). More preferably, the first peak (P1) is comprised in therange of from 58.0 to 58.5 ppm and the second peak (P2) is comprised inthe range of from −2.5 to −3.8 ppm, wherein the integration of the firstand second peaks offers a ratio of the integration values P1:P2 of1:(0.11-0.13). According to particularly preferred embodiments of thepresent invention, the ²⁷Al MAS NMR of the zeolitic material comprises afirst peak (P1) comprised in the range of from 58.1 to 58.3 ppm and asecond peak (P2) comprised in the range of from −2.7 to −3.6 ppm,preferably in the range of from −2.8 to −3.4 ppm, wherein theintegration of the first and second peaks in the ²⁷Al MAS NMR of thezeolitic material preferably offers a ratio of the integration valuesP1:P2 of 1:(0.115-0.125).

There is no particular restriction according to the present invention asto the state in which the zeolitic material is subject to the ²⁷Al MASNMR experiment. It is however preferred, in particular regarding theintensity of the first and second peaks observed in the ²⁷Al MAS NMRspectrum that the inventive zeolitic material having a CHA-typeframework structure has not been subject to a dealumination treatment oreven more preferably to any treatment susceptible of substantiallyinfluencing the content of framework aluminum present in the zeoliticmaterial ascrystallized. Accordingly, according to a particularlypreferred embodiment of the present invention, the ²⁷Al MAS NMR of thezeolitic material according to any of the particular and preferredembodiments wherein X comprises Al refers to a ²⁷Al MAS NMR spectrum andto the according values obtained therein wherein the zeolitic materialhas not been subject to any post-synthetic treatment and is therefore anuntreated zeolitic material as-crystallized. According to the presentinvention it is, however, further preferred that the ²⁷Al MAS NMR of thezeolitic material according to any of the particular and preferredembodiments wherein X comprises Al refers to a ²⁷Al MAS NMR spectrum andto the according values obtained therein obtained from the zeoliticmaterial as-crystallized wherein after isolation, washing and dryingthereof, the material has only been subject to calcination for removalof the organic template, wherein preferably calcination has beenconducted according to any of the particular and preferred embodimentsas defined in the present application, wherein more preferablycalcination has been conducted at 550° C. for a duration of 5 h underair.

Therefore embodiments of the zeolitic material having a CHA-typeframework structure are preferred according to the present inventionwherein the ²⁷Al MAS NMR of the zeolitic material, and preferably of theuntreated zeolitic material as-crystallized, comprises:

-   -   a first peak (P1) in the range of from 55.0 to 61.5 ppm,        preferably of from 56.0 to 60.5 ppm, more preferably of from        56.5 to 60.0 ppm, more preferably of from 57.0 to 59.5 ppm, more        preferably of from 57.5 to 59.0 ppm, more preferably of from        57.8 to 58.7 ppm, more preferably of from 58.0 to 58.5 ppm, and        even more preferably of from 58.1 to 58.3 ppm; and    -   a second peak (P2) in the range of from −0.0 to −7.0 ppm, more        preferably of from −0.5 to −6.0 ppm, more preferably of from        −1.0 to −5.5 ppm, more preferably of from −1.5 to −5.0 ppm, more        preferably of from −2.0 to −4.5 ppm, more preferably of from        −2.3 to −4.1 ppm, more preferably of from −2.5 to −3.8 ppm, more        preferably of from −2.7 to −3.6 ppm, and even more preferably of        from −2.8 to −3.4 ppm;

wherein the integration of the first and second peaks in the ²⁷Al MASNMR of the zeolitic material preferably offers a ratio of theintegration values P1:P2 comprised in the range of from 1:(0.005-0.17),more preferably of from 1:(0.01-0.16), more preferably of from1:(0.03-0.15), more preferably of from 1:(0.05-0.145), more preferablyof from 1:(0.08-0.14), more preferably of from 1:(0.10-0.135), morepreferably of from 1:(0.11-0.13), and even more preferably of from1:(0.115-0.125).

As regards the ²⁹Si MAS NMR of the inventive zeolitic material havingthe CHA-type framework structure comprising YO₂ wherein Y includes Si oris preferably Si, there is no particular restriction as to the numberand/or respective ppm values and/or relative intensities of the signalsdisplayed in the NMR spectrum. According to the present invention,however, it is preferred that the ²⁹Si MAS NMR comprises:

-   -   a first peak (P′1) in the range of from −102.0 to −106.0 ppm,        and    -   a second peak (P′2) in the range of from −108.0 to −112.5 ppm,

wherein more preferably the integration of the first and second peaks inthe ²⁹Si MAS NMR of the zeolitic material offers a ratio of theintegration values P′1:P′2 comprised in the range of from 0.05 to 0.90.More preferably, the first peak (P′1) is comprised in the range of from−102.5 to −105.5 ppm, and preferably of from −103.0 to −105.0 ppm, andthe second peak (P′2) is in the range of from −109.0 to −111.5 ppm,wherein the integration of the first and second peaks preferably offersa ratio of the integration values P′1:P′2 comprised in the range of from0.10 to 0.70, and preferably of from 0.15 to 0.60. More preferably, thefirst peak (P′1) is comprised in the range of from −103.2 to −104.8 ppm,and preferably of from −103.4 to −104.5 ppm and the second peak (P′2) isin the range of from −109.5 to −111.0 ppm, wherein the integration ofthe first and second peaks preferably offers a ratio of the integrationvalues P′1:P′2 comprised in the range of from 0.20 to 0.50, morepreferably of from 0.25 to 0.45. More preferably, the first peak (P1) iscomprised in the range of from −103.6 to −104.3 ppm, and the second peak(P′2) is in the range of from −110.0 to −110.5 ppm, wherein theintegration of the first and second peaks preferably offers a ratio ofthe integration values P′1:P′2 comprised in the range of from 0.30 to0.40, and more preferably of from 0.32 to 0.38. According to the presentinvention it is however particularly preferred that the ²⁹Si MAS NMR ofthe zeolitic material comprises a first peak (P′1) comprised in therange of from −103.8 to −104.1 ppm and a second peak (P′2) in the rangeof from −110.2 to −110.3 ppm, wherein the integration of the first andsecond peaks in the NMR of the zeolitic material preferably offers aratio of the integration values P′1:P′2 comprised in the range of from0.34 to 0.36.

There is no particular restriction according to the present invention asto the state in which the zeolitic material is subjected to the ²⁹Si MASNMR experiment. It is however preferred that the values given in thepresent application relative to the ²⁹Si MAS NMR spectrum are obtainedfrom the zeolitic material which has not been subject to anypost-synthetic treatment and is therefore an untreated zeolitic materialas-crystallized. According to the present invention it is, however,further preferred that the values given in the present applicationrelative to the ²⁹Si MAS NMR spectrum are directly obtained from thezeolitic material as-crystallized wherein after isolation, washing anddrying thereof, the material has only been subject to calcination forremoval of the organic template, wherein preferably calcination has beenconducted according to any of the particular and preferred embodimentsas defined in the present application, wherein more preferablycalcination has been conducted at 550° C. for a duration of 5 h underair.

Therefore, it is preferred according to the present invention that the²⁹Si MAS NMR of the zeolitic material having a CHA-type frameworkstructure as defined in any of the particular and preferred embodimentsof the present invention comprises:

-   -   a first peak (P′1) in the range of from −102.0 to −106.0 ppm,        preferably of from −102.5 to −105.5 ppm, preferably of from        −103.0 to −105.0 ppm, preferably of from −103.2 to −104.8 ppm,        preferably of from −103.4 to −104.5 ppm, preferably of from        −103.6 to −104.3 ppm, and even more preferably of from −103.8 to        −104.1 ppm; and    -   a second peak (P′2) in the range of from −108.0 to −112.5 ppm,        preferably of from −109.0 to −111.5 ppm, preferably of from        −109.5 to −111.0 ppm, preferably of from −110.0 to −110.5 ppm,        and even more preferably of from −110.2 to −110.3 ppm,

wherein the integration of the first and second peaks in the ²⁹Si MASNMR of the zeolitic material preferably offers a ratio of theintegration values P′1:P′2 comprised in the range of from 0.05 to 0.90,preferably of from 0.10 to 0.70, more preferably of from 0.15 to 0.60,more preferably of from 0.20 to 0.50, more preferably of from 0.25 to0.45, more preferably of from 0.30 to 0.40, more preferably of from 0.32to 0.38, and even more preferably of from 0.34 to 0.36.

There is no particular restriction according to the present invention asto the suitable physical and/or chemical characteristics of theinventive zeolitic materials. Thus, as regards for example the porosityand/or surface area of the inventive materials, these may adopt anysuitable values. Thus, as regards the BET surface area of the zeoliticmaterials as determined according to DIN 66135, it may accordingly rangeanywhere from 100 to 850 m²/g, wherein preferably the surface area ofthe inventive zeolitic materials is comprised in the range of from 300to 800 m²/g, more preferably from 400 to 750 m²/g, more preferably from500 to 700 m²/g, more preferably from 550 to 650 m²/g, and even morepreferably from 580 to 620 m²/g. According to particularly preferredembodiments of the present invention, the BET surface area of thezeolitic materials as determined according to DIN 66135 ranges from 590to 610 m²/g.

In general, there is no particular restriction according to the presentinvention as to the specific type or types of zeolitic materials havinga CHA-type framework which may be contained in the inventive zeoliticmaterial. It is, however, preferred that the inventive zeolitic materialcomprises one or more zeolites selected from the group consisting of(Ni(deta)₂)-UT-6, Chabazite, |Li—Na|[Al—Si—O]-CHA, DAF-5, Dehyd.Na-Chabazite, K-Chabazite, LZ-218, Linde D, Linde R, Phi, SSZ-62,UiO-21, Willhendersonite, ZK-14, ZYT-6, and combinations of two or morethereof. More preferably the inventive zeolitic material having aCHA-type framework structure comprises one or more zeolites selectedfrom the group consisting of (Ni(deta)₂)-UT-6, Chabazite,|Li—Na|[Al—Si—O]-CHA, DAF-5, Dehyd. Na-Chabazite, K-Chabazite (Iran),LZ-218, Linde D, Linde R, Phi, SSZ-62, UiO-21, Willhendersonite, ZK-14,ZYT-6, and combinations of two or more thereof. According toparticularly preferred embodiments of the present invention, theinventive zeolitic material comprises Chabazite, wherein even morepreferably the inventive zeolitic material according to particular andpreferred embodiments of the present invention is Chabazite.

Depending on the specific needs of its application, the zeoliticmaterial of the present invention can be employed as such, like in theform of a powder, a spray powder or a spray granulate obtained fromabove-described separation techniques, e.g. decantation, filtration,centrifugation, or spraying.

In many industrial applications, it is often desired on the part of theuser not to employ the zeolitic material as powder or sprayed material,i.e. the zeolitic material obtained by the separation of the materialfrom its mother liquor, optionally including washing and drying, andsubsequent calcination, but a zeolitic material which is furtherprocessed to give moldings. Such moldings are required particularly inmany industrial processes, e.g. in many processes wherein the zeoliticmaterial of the present invention is employed as catalyst or adsorbent.

Accordingly, the present invention also relates to a molding comprisingthe inventive zeolitic material.

In general, the powder or sprayed material can be shaped without anyother compounds, e.g. by suitable compacting, to obtain moldings of adesired geometry, e.g. tablets, cylinders, spheres, or the like.

Preferably, the powder or sprayed material is admixed with or coated bya suitable refractory binder. In general, suitable binders are allcompounds which impart adhesion and/or cohesion between the zeoliticmaterial particles to be bonded which goes beyond the physisorptionwhich may be present without a binder. Examples of such binders aremetal oxides, such as, for example, SiO₂, Al₂O₃, TiO₂, ZrO₂ or MgO orclays, or mixtures of two or more of these compounds.

Naturally occurring clays which can be employed include themontmorillonite and kaolin family, which families include thesubbentonites, and the kaolins commonly known as Dixie, McNamee, Georgiaand Florida clays or others in which the main mineral constituent ishalloysite, kaolinite, dickite, nacrite, or anauxite. Such clays can beused in the raw state as originally mined or initially subjected tocalcination, acid treatment or chemical modification. In addition, thezeolitic material according to the present invention can be compositedwith a porous matrix material such as silica-alumina, silica-magnesia,silica-zirconia, silica-thoria, silica-beryllia and silica-titania aswell as ternary compositions such as silica-alumina-thoria,silica-alumina-zirconia, silica-alumina-magnesia andsilica-magnesia-zirconia.

The zeolitic material of the present invention may therefore also beprovided in the form of extrudates, pellets, tablets or particles of anyother suitable shape, for use as a packed bed of particulate catalyst,or as shaped pieces such as plates, saddles, tubes, or the like.

Also preferably, the powder or the sprayed material, optionally afteradmixing or coating by a suitable refractory binder as described above,is formed into a slurry, for example with water, which is deposited upona suitable refractory carrier. The slurry may also comprise othercompounds such as, e.g., stabilizers, defoamers, promoters, or the like.Typically, the carrier comprises a member, often referred to as a“honeycomb” carrier, comprising one or more refractory bodies having aplurality of fine, parallel gas flow passages extending there through.Such carriers are well known in the art and may be made of any suitablematerial such as cordierite or the like.

In general, the zeolitic material described above can be used asmolecular sieve, adsorbent, catalyst, catalyst support or binderthereof. For example, the zeolitic material can be used as molecularsieve to dry gases or liquids, for selective molecular separation, e.g.for the separation of hydrocarbons or amines; as ion exchanger; aschemical carrier; as adsorbent, in particular as adsorbent for theseparation of hydrocarbons or amines; or as a catalyst. Most preferably,the zeolitic material according to the present invention is used as acatalyst and/or as a catalyst support.

According to a preferred embodiment of the present invention, thezeolitic material of the invention is used in a catalytic process,preferably as a catalyst and/or catalyst support, and more preferably asa catalyst. In general, the zeolitic material of the invention can beused as a catalyst and/or catalyst support in any conceivable catalyticprocess, wherein processes involving the conversion of at least oneorganic compound is preferred, more preferably of organic compoundscomprising at least one carbon-carbon and/or carbon-oxygen and/orcarbon-nitrogen bond, more preferably of organic compounds comprising atleast one carbon-carbon and/or carbon-oxygen bond, and even morepreferably of organic compounds comprising at least one carbon-carbonbond. In particularly preferred embodiments of the present invention,the zeolitic material is used as a catalyst and/or catalyst support in afluid catalytic cracking (FCC) process.

Furthermore, it is preferred according to the present invention, thatthe zeolitic material is used as a catalyst for producing light olefinsfrom non-petroleum feedstock by conversion of oxygenates, such as loweralcohols (methanol, ethanol), ethers (dimethyl ether, methyl ethylether), esters (dimethyl carbonate, methyl formate) and the like toolefins, and especially in the conversion of lower alcohols to lightolefins. According to particularly preferred embodiments, the zeoliticmaterial of the present invention is used in the conversion of methanolto olefin (MTO)

According to a further embodiment of the present invention, the zeoliticmaterial of the invention is preferably used in a catalytic processinvolving the conversion of at least one compound comprising at leastone nitrogen-oxygen bond. Particularly preferred according to thepresent invention is the use of the zeolitic material as a catalystand/or catalyst support in a selective catalytic reduction (SCR) processfor the selective reduction of nitrogen oxides NO_(x); for the oxidationof NH₃, in particular for the oxidation of NH₃ slip in diesel systems;for the decomposition of N₂O. According to particularly preferredembodiments of the present invention, the zeolitic material used in acatalytic process involving the conversion of at least one compoundcomprising at least one nitrogen-oxygen bond comprises Cu and/or Fe, andmore preferably Cu.

Therefore, the present invention also relates to a method forselectively reducing nitrogen oxides NO_(x) by contacting a streamcontaining NO_(x) with a catalyst containing the zeolitic materialaccording to the present invention under suitable reducing conditions;to a method of oxidizing NH₃, in particular of oxidizing NH₃ slip indiesel systems, by contacting a stream containing NH₃ with a catalystcontaining the zeolitic material according to the present inventionunder suitable oxidizing conditions; to a method of decomposing of N₂Oby contacting a stream containing N₂O with a catalyst containing thezeolitic material according to the present invention under suitabledecomposition conditions; to a method of controlling emissions inAdvanced Emission Systems such as Homogeneous Charge CompressionIgnition (HCCI) engines by contacting an emission stream with a catalystcontaining the zeolitic material according to the present inventionunder suitable conditions; to a fluid catalytic cracking FCC processwherein the zeolitic material according to the present invention isemployed as additive; to a method of converting an organic compound bycontacting said compound with a catalyst containing the zeoliticmaterial according to the present invention under suitable conversionconditions; to a “stationary source” process wherein a catalyst isemployed containing the zeolitic material according to the presentinvention.

Therefore, the present invention also relates to a method forselectively reducing nitrogen oxides NO_(x), wherein a gaseous streamcontaining nitrogen oxides NO_(x), preferably also containing ammoniaand/urea, is contacted with the zeolitic material according to thepresent invention or the zeolitic material obtainable or obtainedaccording to the present invention, preferably in the form of a moldedcatalyst, still more preferably as a molded catalyst wherein thezeolitic material is deposited on a suitable refractory carrier, stillmore preferably on a “honeycomb” carrier.

The nitrogen oxides which are reduced using a catalyst containing thezeolitic material according to the present invention or the zeoliticmaterial obtainable or obtained according to the present invention maybe obtained by any process, e.g. as a waste gas stream. Among others,waste gas streams as obtained in processes for producing adipic acid,nitric acid, hydroxylamine derivatives, caprolactame, glyoxal,methyl-glyoxal, glyoxylic acid or in processes for burning nitrogenousmaterials may be mentioned.

Most preferably, the zeolitic material according to the presentinvention or the zeolitic material obtainable or obtained according tothe present invention is used as a molded catalyst, still morepreferably as a molded catalyst wherein the zeolitic material isdeposited on a suitable refractory carrier, still more preferably on a“honeycomb” carrier, for the selective reduction of nitrogen oxidesNO_(x), i.e. for selective catalytic reduction of nitrogen oxides. Inparticular, the selective reduction of nitrogen oxides wherein thezeolitic material according to the present invention is employed ascatalytically active material is carried out in the presence ammonia orurea. While ammonia is the reducing agent of choice for stationary powerplants, urea is the reducing agent of choice for mobile SCR systems.Typically, the SCR system is integrated in the engine and vehicle designand, also typically, contains the following main components: SCRcatalyst containing the zeolitic material according to the presentinvention; a urea storage tank; a urea pump; a urea dosing system; aurea injector/nozzle; and a respective control unit.

Furthermore, it is preferred according to the present invention that thezeolitic material is used as a molecular trap for organic compounds. Ingeneral, any type of organic compound may be trapped in the zeoliticmaterial, wherein it is preferred that the compound is reversiblytrapped, such that it may be later released from the zeolitic material,preferably wherein the organic compound is released—preferably withoutconversion thereof—by an increase in temperature and/or a decrease inpressure. Furthermore, it is preferred that the zeolitic material isused to trap organic compounds of which the dimensions allow them topenetrate the microporous system of the molecular structure. Accordingto yet further embodiments of the present invention, it is preferredthat the trapped compounds are released under at least partialconversion thereof to a chemical derivative and/or to a decompositionproduct thereof, preferably to a thermal decomposition product thereof.

When preparing specific catalytic compositions or compositions fordifferent purposes, it is also conceivable to blend the zeoliticmaterial according to the present invention with at least one othercatalytically active material or a material being active with respect tothe intended purpose. It is also possible to blend at least twodifferent inventive materials which may differ in their YO₂:X₂O₃ molarratio, and in particular in their SiO₂:Al₂O₃ molar ratio, and/or in thepresence or absence of one or more further metals such as one or moretransition metals and/or in the specific amounts of a further metal suchas a transition metal, wherein according to particularly preferredembodiments, the one or more transition metal comprises Cu and/or Fe,more preferably Cu. It is also possible to blend at least two differentinventive materials with at least one other catalytically activematerial or a material being active with respect to the intendedpurpose.

Also, the catalyst may be disposed on a substrate. The substrate may beany of those materials typically used for preparing catalysts, and willusually comprise a ceramic or metal honeycomb structure. Any suitablesubstrate may be employed, such as a monolithic substrate of the typehaving fine, parallel gas flow passages extending there through from aninlet or an outlet face of the substrate, such that passages are open tofluid flow there through (referred to as honeycomb flow throughsubstrates). The passages, which are essentially straight paths fromtheir fluid inlet to their fluid outlet, are defined by walls on whichthe catalytic material is disposed as a washcoat so that the gasesflowing through the passages contact the catalytic material. The flowpassages of the monolithic substrate are thin-walled channels, which canbe of any suitable cross-sectional shape and size such as trapezoidal,rectangular, square, sinusoidal, hexagonal, oval, circular, etc. Suchstructures may contain from about 60 to about 400 or more gas inletopenings (i.e., cells) per square inch (2.54 cm×2.54 cm) of crosssection.

The substrate can also be a wall-flow filter substrate, where thechannels are alternately blocked, allowing a gaseous stream entering thechannels from one direction (inlet direction), to flow through thechannel walls and exit from the channels from the other direction(outlet direction). The catalyst composition can be coated on the flowthrough or wall-flow filter. If a wall flow substrate is utilized, theresulting system will be able to remove particulate matter along withgaseous pollutants. The wall-flow filter substrate can be made frommaterials commonly known in the art, such as cordierite, aluminumtitanate or silicon carbide. It will be understood that the loading ofthe catalytic composition on a wall flow substrate will depend onsubstrate properties such as porosity and wall thickness, and typicallywill be lower than loading on a flow through substrate.

The ceramic substrate may be made of any suitable refractory material,e.g., cordierite, cordierite-alumina, silicon nitride, zircon mullite,spodumene, alumina-silica magnesia, zircon silicate, sillimanite, amagnesium silicate, zircon, petalite, alpha-alumina, an aluminosilicate,and the like.

The substrates useful for the catalysts of embodiments of the presentinvention may also be metallic in nature and be composed of one or moremetals or metal alloys. The metallic substrates may be employed invarious shapes such as corrugated sheet or monolithic form. Suitablemetallic supports include the heat resistant metals and metal alloyssuch as titanium and stainless steel as well as other alloys in whichiron is a substantial or major component. Such alloys may contain one ormore of nickel, chromium and/or aluminum, and the total amount of thesemetals may advantageously comprise at least 15 wt. % of the alloy, e.g.,10-25 wt. % of chromium, 3-8 wt. % of aluminum and up to 20 wt. % ofnickel. The alloys may also contain small or trace amounts of one ormore other metals such as manganese, copper, vanadium, titanium, and thelike. The surface or the metal substrates may be oxidized at hightemperatures, e.g., 1000° C. and higher, to improve the resistance tocorrosion of the alloys by forming an oxide layer on the surfaces of thesubstrates. Such high temperature-induced oxidation may enhance theadherence of the refractory metal oxide support and catalyticallypromoting metal components to the substrate.

In alternative embodiments, zeolitic material according to the presentinvention may be deposited on an open cell foam substrate. Suchsubstrates are well known in the art, and are typically formed ofrefractory ceramic or metallic materials.

Especially preferred is the use of a catalyst containing the zeoliticmaterial according to the present invention or the zeolitic materialobtainable or obtained according to the present invention for removal ofnitrogen oxides NO_(x) from exhaust gases of internal combustionengines, in particular diesel engines, which operate at combustionconditions with air in excess of that required for stoichiometriccombustion, i.e., lean.

Therefore, the present invention also relates to a method for removingnitrogen oxides NO_(x) from exhaust gases of internal combustionengines, in particular diesel engines, which operate at combustionconditions with air in excess of that required for stoichiometriccombustion, i.e., at lean conditions, wherein a catalyst containing thezeolitic material according to the present invention or the zeoliticmaterial obtainable or obtained according to the present invention isemployed as catalytically active material.

The present invention therefore relates to the use of the zeoliticmaterial of the invention, in particular in the field of catalysisand/or in the treatment of exhaust gas, wherein said exhaust gastreatment comprises industrial and automotive exhaust gas treatment. Inthese and other applications, the zeolitic material of the presentinvention can by way of example be used as a molecular sieve, catalyst,and/or catalyst support.

In embodiments of the present invention involving the use of thezeolitic material of the invention in exhaust gas treatment, thezeolitic material is preferably used in the treatment of industrial orautomotive exhaust gas, more preferably as a molecular sieve in saidapplications. In a particularly preferred embodiment, the zeoliticmaterial used in exhaust gas treatment is comprised in a hydrocarbontrap.

Therefore, the present invention further relates to the use of azeolitic material according to the present invention, and in particularaccording to preferred and particularly preferred embodiments thereof asdefined in the present application, as a molecular sieve, as anadsorbent, for ion-exchange, as a catalyst and/or as a catalyst support,preferably as a catalyst for the selective catalytic reduction (SCR) ofnitrogen oxides NO_(x); for the oxidation of NH₃, in particular for theoxidation of NH₃ slip in diesel systems; for the decomposition of N₂O;as an additive in fluid catalytic cracking (FCC) processes; and/or as acatalyst in organic conversion reactions, preferably in the conversionof alcohols to olefins, and more preferably in methanol to olefin (MTO)catalysis. According to the present invention it is however particularpreferred that the organo-template-free zeolitic material having aCHA-type framework structure is used as a catalyst for the selectivecatalytic reduction (SCR) of nitrogen oxides NO_(x).

The present invention includes the following embodiments, wherein theseinclude the specific combinations of embodiments as indicated by therespective interdependencies defined therein;

-   1. A process for the preparation of a zeolitic material having a    CHA-type framework structure comprising YO₂ and X₂O₃, wherein said    process comprises the steps of:    -   (1) providing a mixture comprising one or more sources for YO₂,        one or more sources for X₂O₃, one or more tetraalkylammonium        cation R¹R²R³R⁴N⁺-containing compounds, and one or more        tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing compounds as        structure directing agent;    -   (2) crystallizing the mixture obtained in step (1) for obtaining        a zeolitic material having a CHA-type framework structure;    -   wherein Y is a tetravalent element and X is a trivalent element,    -   wherein R¹, R², R³, R⁴, R⁵, R⁶, and R⁷ independently from one        another stand for alkyl, and    -   wherein R⁸ stands for cycloalkyl.-   2. The process of embodiment 1, wherein the mixture provided in    step (1) preferably does not contain any substantial amount of a    source for Z₂O₅, wherein Z is P, preferably P and As, wherein more    preferably Z is any pentavalent element which is a source for Z₂O₅    in the CHA-type framework structure crystallized in step (2).-   3. The process of embodiment 1 or 2, wherein R¹, R², R³, R⁴, R⁵, R⁶,    and R⁷ independently from one another stand for optionally    substituted and/or optionally branched (C₁-C₆)alkyl, preferably    (C₁-C₅)alkyl, more preferably (C₁-C₄)alkyl, more preferably    (C₁-C₃)alkyl, and even more preferably for optionally substituted    methyl or ethyl, wherein even more preferably R¹, R², R³, R⁴, R⁵,    R⁶, and R⁷ stand for optionally substituted methyl, preferably    unsubstituted methyl.-   4. The process of any of embodiments 1 to 3, wherein R⁸ stands for    optionally heterocyclic and/or optionally substituted 5- to    8-membered cycloalkyl, preferably for 5- to 7-membered cycloalkyl,    more preferably for 5- or 6-membered cycloalkyl, wherein even more    preferably R⁸ stands for optionally heterocyclic and/or optionally    substituted 6-membered cycloalkyl, preferably optionally substituted    cyclohexyl, and more preferably non-substituted cyclohexyl.-   5. The process of any of embodiments 1 to 4, wherein the one or more    tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing compounds comprise    one or more N,N,N-tri(C₁-C₄)alkyl-(C₅-C₇)cycloalkylammonium    compounds, preferably one or more    N,N,N-tri(C₁-C₃)alkyl-(C₅-C₆)cycloalkylammonium compounds, more    preferably one or more    N,N,N-tri(C₁-C₂)alkyl-(C₅-C₆)cycloalkylammonium compounds, more    preferably one or more N,N,N-tri(C₁-C₂)alkyl-cyclopentylammonium    and/or one or more N,N,N-tri(C₁-C₂)alkyl-cyclohexylammonium    compounds, more preferably one or more compounds selected from    N,N,N-triethyl-cyclohexylammonium,    N,N-diethyl-N-methyl-cyclohexylammonium,    N,N-dimethyl-N-ethyl-cyclohexylammonium,    N,N,N-trimethyl-cyclohexylammonium compounds, and mixtures of two or    more thereof, wherein more preferably the one or more    tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing compounds comprise    one or more N,N,N-trimethyl-cyclohexylammonium compounds, and    wherein more preferably the one or more tetraalkylammonium cation    R⁵R⁶R⁷R⁸N⁺-containing compounds consist of one or more    N,N,N-trimethyl-cyclohexylammonium compounds.-   6. The process of any of embodiments 1 to 5, wherein the one or more    tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compounds comprise    one or more compounds selected from the group consisting of    tetra(C₁-C₆)alkylammonium compounds, preferably    tetra(C₁-C₅)alkylammonium compounds, more preferably    tetra(C₁-C₄)alkylammonium compounds, and more preferably    tetra(C₁-C₃)alkylammonium compounds, wherein independently from one    another the alkyl substituents are optionally substituted and/or    optionally branched, and wherein more preferably the one or more    tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compounds are    selected from the group consisting of optionally substituted and/or    optionally branched tetrapropylammonium compounds,    ethyltripropylammonium compounds, diethyldipropylammonium compounds,    triethylpropylammonium compounds, methyltripropylammonium compounds,    dimethyldipropylammonium compounds, trimethylpropylammonium    compounds, tetraethylammonium compounds, triethylmethylammonium    compounds, diethyldimethylammonium compounds, ethyltrimethylammonium    compounds, tetramethylammonium compounds, and mixtures of two or    more thereof, preferably from the group consisting of optionally    substituted and/or optionally branched tetraethylammonium compounds,    triethylmethylammonium compounds, diethyldimethylammonium compounds,    ethyltrimethylammonium compounds, tetramethylammonium compounds, and    mixtures of two or more thereof, preferably from the group    consisting of optionally substituted tetramethylammonium compounds,    wherein more preferably the one or more tetraalkylammonium cation    R¹R²R³R⁴N⁺-containing compounds comprises one or more    tetramethylammonium compounds, and wherein more preferably the one    or more tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compounds    consists of one or more tetramethylammonium compounds.-   7. The process of any of embodiments 1 to 6, wherein the one or more    tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compounds and/or the    one or more tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing    compounds are salts, preferably one or more salts selected from the    group consisting of halides, preferably chloride and/or bromide,    more preferably chloride, hydroxide, sulfate, nitrate, phosphate,    acetate, and mixtures of two or more thereof, more preferably from    the group consisting of chloride, hydroxide, sulfate, and mixtures    of two or more thereof, wherein more preferably the one or more    tetraalkylammonium cation R¹R²R³R⁴N⁺-containing compounds and/or the    one or more tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing    compounds are tetraalkylammonium hydroxides and/or chlorides, and    even more preferably tetraalkylammonium hydroxides.-   8. The process of any of embodiments 1 to 7 wherein Y is selected    from the group consisting of Si, Sn, Ti, Zr, Ge, and mixtures of two    or more thereof, Y preferably being Si.-   9. The process of any of embodiments 1 to 8, wherein the one or more    sources for YO₂ comprises one or more compounds selected from the    group consisting of fumed silica, silica hydrosols, reactive    amorphous solid silicas, silica gel, silicic acid, water glass,    sodium metasilicate hydrate, sesquisilicate, disilicate, colloidal    silica, silicic acid esters, and mixtures of two or more thereof,    preferably from the group consisting of fumed silica, silica    hydrosols, reactive amorphous solid silicas, silica gel, silicic    acid, colloidal silica, silicic acid esters, and mixtures of two or    more thereof, more preferably from the group consisting of fumed    silica, silica hydrosols, reactive amorphous solid silicas, silica    gel, colloidal silica, and mixtures of two or more thereof, wherein    even more preferably the one or more sources for YO₂ comprises fumed    silica and/or colloidal silica, preferably colloidal silica.-   10. The process of any of embodiments 1 to 9, wherein X is selected    from the group consisting of Al, B, In, Ga, and mixtures of two or    more thereof, X preferably being Al and/or B, and more preferably    being Al.-   11. The process of any of embodiments 1 to 10, wherein the one or    more sources for X₂O₃ comprises one or more compounds selected from    the group consisting of alumina, aluminates, aluminum salts, and    mixtures of two or more thereof, preferably from the group    consisting of alumina, aluminum salts, and mixtures of two or more    thereof, more preferably from the group consisting of alumina,    aluminum tri(C₁-C₅)alkoxide, AlO(OH), Al(OH)₃, aluminum halides,    preferably aluminum fluoride and/or chloride and/or bromide, more    preferably aluminum fluoride and/or chloride, and even more    preferably aluminum chloride, aluminum sulfate, aluminum phosphate,    aluminum fluorosilicate, and mixtures of two or more thereof, more    preferably from the group consisting of aluminum tri(C₂-C₄)alkoxide,    AlO(OH), Al(OH)₃, aluminum chloride, aluminum sulfate, aluminum    phosphate, and mixtures of two or more thereof, more preferably from    the group consisting of aluminum tri(C₂-C₃)alkoxide, AlO(OH),    Al(OH)₃, aluminum chloride, aluminum sulfate, and mixtures of two or    more thereof, more preferably from the group consisting of aluminum    tripropoxides, AlO(OH), aluminum sulfate, and mixtures of two or    more thereof, wherein more preferably the one or more sources for    X₂O₃ comprises aluminum triisopropoxide, and wherein even more    preferably the one or more sources for X₂O₃ consists of aluminum    triisopropoxide.-   12. The process of any of embodiments 1 to 11, wherein the mixture    according to step (1) further comprises one or more solvents,    wherein said one or more solvents preferably comprises water,    preferably distilled water, wherein more preferably water is    contained as the one or more solvents in the mixture according to    step (1), preferably distilled water.-   13, The process of any of embodiments 1 to 12, wherein the molar    ratio of the one or more tetraalkylammonium cations R¹R²R³R⁴N⁺:YO₂    in the mixture provided according to step (1) ranges from 0.005 to    0.5, preferably from 0.01 to 0.25, more preferably from 0.03 to 0.2,    more preferably from 0.05 to 0.15, more preferably from 0.07 to    0.12, more preferably from 0.08 to 0.1, and even more preferably    from 0.085 to 0.010.-   14. The process of any of embodiments 1 to 13, wherein the molar    ratio of the one or more tetraalkylammonium cations R⁵R⁶R⁷R⁸N⁺:YO₂    in the mixture provided according to step (1) ranges from 0.001 to    2.0, preferably from 0.005 to 1.0, more preferably from 0.01 to 0.5,    more preferably from 0.03 to 0.3, more preferably from 0.05 to 0.25,    more preferably from 0.07 to 0.22, more preferably from 0.08 to 0.2,    more preferably from 0.09 to 0.19, and even more preferably from    0.10 to 0.18.-   15. The process of any of embodiments 1 to 14, wherein the molar    ratio R¹R²R³R⁴N⁺:R⁵R⁶R⁷R⁸N⁺ of the one or more tetraalkylammonium    cations R¹R²R³R⁴N⁺ to the one or more tetraalkylammonium cations    R⁵R⁶R⁷R⁸N⁺ in the mixture provided according to step (1) ranges from    0.01 to 5, preferably from 0.05 to 2, more preferably from 0.1 to    1.5, more preferably from 0.2 to 1.2, more preferably from 0.3 to    1.1, more preferably from 0.4 to 0.1, more preferably from 0.45 to    0.65, and even more preferably from 0.5 to 0.9.-   16. The process of any of embodiments 1 to 15, wherein the    crystallization in step (2) involves heating of the mixture,    preferably at a temperature ranging from 90 to 250° C., preferably    from 100 to 220° C., more preferably from 130 to 200° C., more    preferably from 150 to 190° C., more preferably from 160 to 180° C.,    and even more preferably from 165 to 175° C.-   17. The process of any of embodiments 1 to 16, wherein the    crystallization in step (2) is conducted under solvothermal    conditions, preferably under hydrothermal conditions.-   18. The process of any of embodiments 1 to 17, wherein the    crystallization in step (2) involves heating of the mixture for a    period ranging from 3 to 40 h, preferably from 5 to 30 h, more    preferably from 8 to 25 h, more preferably from 10 to 21 h, more    preferably from 13 to 20 h, and even more preferably from 15 to 20    h.-   19. The process of any of embodiments 1 to 18, wherein the    crystallization in step (2) involves agitating the mixture,    preferably by stirring.-   20. The process of any of embodiments 1 to 19 further comprising one    or more of the following steps of    -   (3) isolating the zeolitic material, preferably by filtration,        and/or    -   (4) washing the zeolitic material, and/or    -   (5) drying and/or calcining the zeolitic material, and/or    -   (6) subjecting the zeolitic material to an ion-exchange        procedure,    -   wherein the steps (3) and/or (4) and/or (5) and/or (6) can be        conducted in any order, and    -   wherein one or more of said steps is preferably repeated one or        more times.-   21. The process of embodiment 20, wherein in the at least one    step (6) one or more ionic non-framework elements contained in the    zeolite framework is ion-exchanged, preferably against one or more    cations and/or cationic elements, wherein the one or more cation    and/or cationic elements are preferably selected from the group    consisting of H⁺, NH₄ ⁺, Sr, Zr, Cr, Mg, Mo, Fe, Co, Ni, Cu, Zn, Ru,    Rh, Pd, Ag, Os, Ir, Pt, Au, and mixtures of two or more thereof,    more preferably from the group consisting of H⁺, NH₄ ⁺, Sr, Cr, Mo,    Fe, Co, Ni, Cu, Zn, Ag, and mixtures of two or more thereof, more    preferably from the group consisting of H⁺, NH₄ ⁺, Cr, Mg, Mo, Fe,    Ni, Cu, Zn, Ag, and mixtures of two or more thereof, more preferably    from the group consisting of Mg, Mo, Fe, Ni, Cu, Zn, Ag, and    mixtures of two or more thereof, wherein more preferably the one or    more cation and/or cationic elements comprise Cu and/or Fe,    preferably Cu, wherein even more preferably the one or more cation    and/or cationic elements consist of Cu and/or Fe, preferably of Cu,    and    -   wherein the one or more ionic non-framework elements preferably        comprise H⁺ and/or an alkali metal, the alkali metal preferably        being selected from the group consisting of Li, Na, K, Cs, and        combinations of two or more thereof, more preferably from the        group consisting of Li, Na, K, and combinations of two or more        thereof, wherein more preferably the alkali metal is Na and/or        K, even more preferably Na.-   22. The process of any of embodiments 1 to 21, wherein the mixture    provided in step (1) does not contain any substantial amount of a    trimethyl benzyl ammonium containing compound, preferably of a    trialkyl benzyl ammonium compound wherein preferably the mixture    provided in step (1) does not contain any substantial amount of an    organotemplate other than the one or more tetraalkylammonium cation    R⁵R⁶R⁷R⁸N⁺-containing compounds as structure directing agent,    wherein more preferably the mixture provided in step (1) does not    contain any substantial amount of a structure directing agent other    than the one or more tetraalkylammonium cation R⁵R⁶R⁷R⁸N⁺-containing    compounds, and wherein even more preferably, the mixture provided in    step (1) only contains one or more    N,N,N-trimethyl-cyclohexylammonium compounds and preferably    N,N,N-trimethyl-cyclohexylammonium hydroxide as structure directing    agent for the crystallization of a zeolitic material having a    CHA-type framework structure in step (2).-   23. The process of any of embodiments 1 to 22, wherein the mixture    provided in step (1) further comprises seed crystals, preferably    seed crystals comprising a zeolitic material having the CHA-type    framework structure, wherein the zeolitic material of the seed    crystals is preferably obtainable and/or obtained according to any    one of embodiments 1 to 22.-   24. The process of embodiment 23, wherein the amount of seed    crystals in the mixture according to step (1) ranges from 0.1 to 20    wt.-% based on 100 wt.-% of YO₂ in the at least one source for YO₂,    preferably from 0.5 to 15 wt.-%, more preferably from 1 to 12 wt.-%,    more preferably from 1.5 to 10 wt.-%, more preferably from 2 to 8    wt.-%, more preferably from 2.5 to 6 wt.-%, more preferably from 3    to 5 wt.-%, and even more preferably from 3.5 to 4.5 wt.-% based on    100 wt.-% of YO₂.-   25. A synthetic zeolitic material having a CHA-type framework    structure obtainable and/or obtained according to the process of any    of embodiments 1 to 24.-   26. A synthetic zeolitic material having a CHA-type framework    structure, preferably obtainable and/or obtained according to the    process of any of embodiments 1 to 24, wherein the CHA-type    framework structure comprises YO₂ and X₂O₃, wherein Y is a    tetravalent element and X is a trivalent element, and wherein the    IR-spectrum of the zeolitic material comprises:    -   a first absorption band (B1) in the range of from 3,720 to 3,740        cm⁻¹; and    -   a second absorption band (B2) in the range of from 1,850 to        1,890 cm⁻¹;    -   wherein the ratio of the maximum absorbance of the first        absorption band to the second absorption band B1:B2 is comprised        in the range of from 0.5 to 1.55, preferably from 0.8 to 1.45,        more preferably from 1.0 to 1.4, more preferably from 1.1 to        1.38, more preferably from 1.2 to 1.37, more preferably from 1.3        to 1.36, and more preferably from 1.33 to 1.35.-   27. The zeolitic material of embodiment 26, wherein the particle    size D10 of the zeolitic material is comprised in the range of from    500 to 2,500 nm, preferably from 600 to 2,000 nm, more preferably    from 800 to 1,800 nm, more preferably from 1,000 to 1,600 nm, more    preferably from 1,200 to 1,500 nm, and more preferably from 1,300 to    1,400 nm.-   28. The zeolitic material of embodiment 26, wherein the average    particle size D50 of the zeolitic material is comprised in the range    of from 700 to 3,500 nm, preferably from 900 to 3,000 nm, more    preferably from 1,100 to 2,800 nm, more preferably from 1,300 to    2,500 nm, more preferably from 1,500 to 2,200 nm, more preferably    from 1,550 to 2,000 nm, more preferably from 1,600 to 1,900 nm, and    more preferably from 1,650 to 1,850 nm.-   29. The zeolitic material of embodiment 26, wherein the particle    size D90 of the zeolitic material is comprised in the range of from    900 to 4,500 nm, preferably from 1,100 to 4,000 nm, more preferably    from 1,400 to 3,800 nm, more preferably from 1,600 to 3,500 nm, more    preferably from 1,800 to 3,200 nm, more preferably from 2,000 to    2,900 nm, more preferably from 2,100 to 2,700 nm, more preferably    from 2,200 to 2,600 nm, more preferably from 2,250 to 2,550 nm, and    more preferably from 2,300 to 2,500 nm.-   30. The zeolitic material of embodiment 26, wherein the particle    size D10 of the zeolitic material is comprised in the range of from    1,200 to 1,500 nm, more preferably from 1,250 to 1,450 nm, and more    preferably from 1,300 to 1,400 nm,    -   wherein the average particle size D50 of the zeolitic material        is comprised in the range of from 1,550 to 1,950 nm, preferably        from 1,600 to 1,900 nm, and more preferably from 1,650 to 1,850        nm, and    -   wherein the particle size D90 of the zeolitic material is        comprised in the range of from 2,000 to 2,900 nm, preferably        from 2,100 to 2,700 nm, more preferably from 2,200 to 2,600 nm,        more preferably from 2,250 to 2,550 nm, and more preferably from        2,300 to 2,500 nm.-   31. The zeolitic material of any of embodiments 26 to 30, wherein    the CHA-type framework does not contain any substantial amount of    the elements P and/or As, preferably one or more elements selected    from the group consisting of P, As, V, and combinations of two or    more thereof, more preferably one or more elements selected from the    group consisting of P, As, Sb, Bi, V, Nb, Ta, and combinations of    two or more thereof, wherein even more preferably said framework    structure does not contain any substantial amount of any pentavalent    elements Z as framework element.-   32. The zeolitic material of any of embodiments 26 to 31, wherein    the ²⁷Al MAS NMR of the zeolitic material comprises:    -   a first peak (P1) in the range of from 55.0 to 61.5 ppm,        preferably of from 56.0 to 60.5 ppm, more preferably of from        56.5 to 60.0 ppm, more preferably of from 57.0 to 59.5 ppm, more        preferably of from 57.5 to 59.0 ppm, more preferably of from        57.8 to 58.7 ppm, more preferably of from 58.0 to 58.5 ppm, and        even more preferably of from 58.1 to 58.3 ppm; and    -   a second peak (P2) in the range of from −0.0 to −7.0 ppm,        preferably of from −0.5 to −6.0 ppm, more preferably of from        −1.0 to −5.5 ppm, more preferably of from −1.5 to −5.0 ppm, more        preferably of from −2.0 to −4.5 ppm, more preferably of from        −2.3 to −4.1 ppm, more preferably of from −2.5 to −3.8 ppm, more        preferably of from −2.7 to −3.6 ppm, and even more preferably of        from −2.8 to −3.4 ppm;    -   wherein the integration of the first and second peaks in the        ²⁷Al MAS NMR of the zeolitic material offers a ratio of the        integration values P1:P2 comprised in the range of from        1:(0.005-0.17), preferably of from 1:(0.01-0.16), more        preferably of from 1:(0.03-0.15), more preferably of from        1:(0.05-0.145), more preferably of from 1:(0.08-0.14), more        preferably of from 1:(0.10-0.135), more preferably of from        1:(0.11-0.13), and even more preferably of from 1:(0.115-0.125).-   33. The zeolitic material of any of embodiments 26 to 32, wherein    the ²⁹Si MAS NMR of the zeolitic material comprises:    -   a first peak (P′1) in the range of from −102.0 to −106.0 ppm,        preferably of from −102.5 to −105.5 ppm, preferably of from        −103.0 to −105.0 ppm, preferably of from −103.2 to −104.8 ppm,        preferably of from −103.4 to −104.5 ppm, preferably of from        −103.6 to −104.3 ppm, and even more preferably of from −103.8 to        −104.1 ppm; and    -   a second peak (P′2) in the range of from −108.0 to −112.5 ppm,        preferably of from −109.0 to −111.5 ppm, preferably of from        −109.5 to −111.0 ppm, preferably of from −110.0 to −110.5 ppm,        and even more preferably of from −110.2 to −110.3 ppm, wherein        the integration of the first and second peaks in the ²⁹Si MAS        NMR of the zeolitic material offers a ratio of the integration        values P′1:P′2 comprised in the range of from 0.05 to 0.90,        preferably of from 0.10 to 0.70, more preferably of from 0.15 to        0.60, more preferably of from 0.20 to 0.50, more preferably of        from 0.25 to 0.45, more preferably of from 0.30 to 0.40, more        preferably of from 0.32 to 0.38, and even more preferably of        from 0.34 to 0.36.-   34. The zeolitic material of any of embodiments 26 to 33, wherein    the CHA-type framework does not contain any substantial amount of P    and/or As, preferably one or more elements selected from the group    consisting of P, As, V, and combinations of two or more thereof,    more preferably one or more elements selected from the group    consisting of P, As, Sb, Bi, V, Nb, Ta, and combinations of two or    more thereof, wherein even more preferably the framework structure    does not contain any substantial amount of any pentavalent elements    Z as framework element, and    -   wherein the zeolitic material preferably does not comprise        SSZ-13 and/or SSZ-15.-   35. The zeolitic material of any of embodiments 26 to 34, wherein    the YO₂:X₂O₃ molar ratio ranges from 4 to 200, preferably from 10 to    100, more preferably from 16 to 60, more preferably from 20 to 40,    more preferably from 23 to 35, and even more preferably from 25 to    30.-   36. The zeolitic material of any of embodiments 26 to 35, wherein Y    is selected from the group consisting of Si, Sn, Ti, Zr, Ge, and    mixtures of two or more thereof, Y preferably being Si.-   37. The zeolitic material of any of embodiments 26 to 36, wherein X    is selected from the group consisting of Al, B, In, Ga, and mixtures    of two or more thereof, X preferably being Al and/or B, and more    preferably being Al.-   38. The zeolitic material of any of embodiments 26 to 37, wherein    the zeolitic material comprises one or more cation and/or cationic    elements as ionic non-framework elements, said one or more cation    and/or cationic elements preferably comprising one or more selected    from the group consisting of H⁺, NH₄ ⁺, Sr, Zr, Cr, Mg, Mo, Fe, Co,    Ni, Cu, Zn, Ru, Rh, Pd, Ag, Os, Ir, Pt, Au, and mixtures of two or    more thereof, more preferably from the group consisting of H⁺, NH₄    ⁺, Sr, Cr, Mo, Fe, Co, Ni, Cu, Zn, Ag, and mixtures of two or more    thereof, more preferably from the group consisting of H⁺, NH₄ ⁺, Cr,    Mg, Mo, Fe, Ni, Cu, Zn, Ag, and mixtures of two or more thereof,    more preferably from the group consisting of Mg, Mo, Fe, Ni, Cu, Zn,    Ag, and mixtures of two or more thereof, wherein more preferably the    one or more cation and/or cationic elements comprise Cu and/or Fe,    preferably Cu, wherein even more preferably the one or more cation    and/or cationic elements consist of Cu and/or Fe, preferably of Cu.-   39. The zeolitic material of embodiment 38, wherein the one or more    cations and/or cationic elements are contained in the zeolitic    material in an amount ranging from 0.01 to 25 wt.-% based on 100    wt.-% of YO₂ comprised in the zeolitic material, preferably from    0.05 to 15.0 wt.-%, more preferably from 0.1 to 10.0 wt.-%, more    preferably from 0.5 to 6.0 wt.-%, more preferably from 1.0 to 4.0    wt.-%, more preferably from 1.5 to 3.5 wt.-%, more preferably from    2.0 to 3.0 wt.-%, more preferably from 2.3 to 2.7 wt.-%.-   40. The zeolitic material of any of embodiments 26 to 39, wherein    the BET surface area of the zeolitic material determined according    to DIN 66135 ranges from 100 to 850 m²/g, preferably from 300 to 800    m²/g, more preferably from 400 to 750 m²/g, more preferably from 500    to 700 m²/g, more preferably from 550 to 650 m²/g, more preferably    from 580 to 620 m²/g, more preferably from 590 to 610 m²/g.-   41. Use of a synthetic zeolitic material having a CHA-type framework    structure according to embodiment 25 to 40 as a molecular sieve, as    an adsorbent, for ion-exchange, or as a catalyst and/or as a    catalyst support, preferably as a catalyst for the selective    catalytic reduction (SCR) of nitrogen oxides NO_(x); for the    oxidation of NH₃, in particular for the oxidation of NH₃ slip in    diesel systems; for the decomposition of N₂O; as an additive in    fluid catalytic cracking (FCC) processes; and/or as a catalyst in    organic conversion reactions, preferably in the conversion of    alcohols to olefins, and more preferably in methanol to olefin (MTO)    catalysis.

DESCRIPTION OF THE FIGURES

FIGS. 1 to 6 display the IR-spectra obtained for the crystallinematerial obtained according to Examples 2 and 3, and ComparativeExamples 1, 2, 3, and 4, respectively. In the figures, the wavenumbersin cm⁻¹ is shown along the abscissa, and the absorbance is plotted alongthe ordinate.

FIG. 7 displays the X-ray diffraction pattern (measured using Cu Kalpha-1 radiation) of the reaction product obtained according toComparative Example 5. For comparative purposes, the line pattern of theCHA type structure is indicated in the diffractogram of the amorphousmaterial as a reference. In the figure, the angle 2 theta in ³ is shownalong the abscissa and the intensities are plotted along the ordinate.

FIG. 8 displays the X-ray diffraction pattern (measured using Cu Kalpha-1 radiation) of the reaction product obtained according toComparative Example 6. In an attempt to identify the reaction product,the line patterns of the hydrogen sodium aluminum silicate structure(H_(1.98)Na_(0.02)Al₂Si₅₀O₁₀₄), of the quartz structure, and of the CHAtype structure are indicated in the diffractogram of the amorphousmaterial as a reference. In the figure, the angle 2 theta in ° is shownalong the abscissa and the intensities are plotted along the ordinate.

EXAMPLES

X-ray diffraction experiments on the powdered materials were performedusing an Advance D8 Series 2 Diffractometer (Bruker/AXS) equipped with aSol-X detector using the Cu K alpha-1 radiation.

²⁷Al MAS solid-state NMR experiments were measured by direct excitationwith 15°-pulse under 10 kHz Magic Angle Spinning using 250 ms recycledelay and 20 ms acquisition. The data was processed with 50 Hzexponential line broadening.

²⁹Si MAS solid-state NMR experiments were performed using a BrukerAvance spectrometer with 300 MHz ¹H Larmor frequency (Bruker Biospin,Germany). Spectra were processed using Bruker Topspin with 30 Hzexponential line broadening, manual phasing, and manual baselinecorrection over the full spectrum width. Spectra were referenced withthe polymer Q8M8 as an external secondary standard, by setting theresonance of the trimethylsilyl M group to 12.5 ppm.

The IR-spectra were obtained from samples free of a carrier material,wherein said sample were heated at 300° C. in high vacuum for 3 h priorto measurement. The measurements were performed using a Nicolet 6700spectrometer in a high vacuum measurement cell with CaF₂ windows. Theobtained data was transformed to absorbance values, and the analysis wasperformed on the spectra after base line correction.

The particle size distribution of the samples was performed bydispersing 0.1 g of the zeolite powder in 100 g H₂O and treating byultrasound for 10 minutes. The dynamic light scattering was performed ona Zetasizer Nano ZS with the Malvern Zeta Sizer Software, Version 634,applying 5 runs à 10 second measurement time for each sample. The givenvalues are the average particle size by number in nanometer.

Example 1 Preparation of a Zeolitic Material having the CHA FrameworkStructure using Trimethylcyclohexylammonium and Tetramethylammonium

692.01 g N,N,N-trimethylcyclohexylammonium hydroxide (20 wt-% solutionin H₂O) were mixed with 56.54 g of aluminiumtriisopropylate and 150.62 gtetramethylammonium hydroxide (25 wt-% solution in H₂O). Afterwards,692.01 g of colloidal silica (LUDOX AS 40; 40 wt.-% colloidal solutionin H₂O) and 11 g of chabazite as seed crystals were added to the stirredmixture. The resulting gel was placed in a stirred autoclave with atotal volume of 2.5 L. The autoclave was heated within 7 h to 170° C.The temperature was kept constant for 30 h. Afterwards the autoclave wascooled down to room temperature. Then, the solids were separated byfiltration and intensive washing with distilled water until thewash-water had a pH of 7. Finally the solid was dried for 10 hours at120° C. to afford 308 g of product which was then calcined at 550° C.for 5 h under air.

The characterization of the material via XRD confirmed the CHA-typeframework structure of the product and afforded an average crystal sizeof 117 nm and a crystallinity of 88%. The material displayed a BETsurface area of 630 m²/g. The elemental analysis prior to calcinationshowed 36 wt-% Si, 2.2 wt-% Al, 11.8 wt-% C, 1.6 wt.-% N and 0.07 wt-%Na in the sample, thus affording an SiO₂:Al₂O₃ atomic ratio (SAR) of 31.

The particle size distribution of the calcined sample afforded a D10value of 1.4 μm, a D50 value of 1.89 μm, and a D90 value of 2.58 μm.

The ²⁹Si MAS NMR of the zeolitic material displays peaks at 103.8 and−110.2 ppm, wherein the integration of the peaks offers relativeintensities of 0.397 and 1 for the signals, respectively.

The ²⁷Al MAS NMR of the zeolitic material displays peaks at 58.3 and−0.7 ppm, wherein the integration of the peaks offers relativeintensities of 1 and 0.112 for the signals, respectively.

Example 2 Preparation of a Zeolitic Material having the CHA FrameworkStructure using Trimethylcyclohexylammonium and Tetramethylammonium

534.54 g N,N,N-trimethylcyclohexylammonium hydroxide (20 wt-% solutionin H₂O) were mixed with 56.54 g of aluminiumtriisopropylate and 150.62 gtetramethylammonium hydroxide (25 wt-% solution in H₂O). Afterwards,692.01 g of colloidal silica (LUDOX AS 40; 40 wt.-% colloidal solutionin H₂O) and 11 g of chabazite as seed crystals were added to the stirredmixture. The resulting gel was placed in a stirred autoclave with atotal volume of 2.5 L. The autoclave was heated within 7 h to 170° C.The temperature was kept constant for 30 h. Afterwards the autoclave wascooled down to room temperature. Then, the solids were separated byfiltration and intensive washing with distilled water until thewash-water had a pH of 7. Finally the solid was dried for 10 hours at120° C. to afford 327 g of product which was then calcined at 550° C.for 5 h for affording 296 g of a white powder.

The characterization of the material via XRD confirmed the CHA-typeframework structure of the product and afforded an average crystal sizeof 117 nm and a crystallinity of 92%. The material displayed a BETsurface area of 613 m²/g, a pore volume of 1.07 cm³/g and a median porewidth of 0.68 nm. The elemental analysis prior to calcination showed 36wt-% Si, 2.9 wt-% Al, 12.9 wt-% C, 1.6 wt.-% N and 0.13 wt-% Na in thesample, thus affording an SiO₂:Al₂O₃ atomic ratio (SAR) of 25.

The IR-spectrum of the calcined sample is shown in FIG. 1, whereinamongst others absorption bands having maxima at 3,732 cm⁻¹ and 1,866cm⁻¹ may be seen, which display a ratio of maximum absorption of theformer to the latter of 1.33.

The particle size distribution of the calcined sample afforded a D10value of 1.3 μm, a D50 value of 1.69 μm, and a D90 value of 2.25 μm.

The ²⁹Si MAS NMR of the zeolitic material displays peaks at −104.1 and−110.3 ppm, wherein the integration of the peaks offers relativeintensities of 0.334 and 1 for the signals, respectively.

The ²⁷Al MAS NMR of the zeolitic material displays peaks at 58.3 and−6.3 ppm, wherein the integration of the peaks offers relativeintensities of 1 and 0.124 for the signals, respectively.

Example 3 Preparation of a Zeolitic Material having the CHA FrameworkStructure using Trimethylcyclohexylammonium and Tetramethylammonium

276.8 kg N,N,N-trimethylcyclohexylammoniumhydroxide (20 wt-% solution inH₂O) were mixed with 34.80 kg of aluminiumtriisopropylate and 77.99 kgtetramethylammonium hydroxide (25 wt-% solution in H₂O). Afterwards,358.32 kg of colloidal silica (LUDOX AS 40; 40 wt-% colloidal solutionin H₂O) and 5.73 kg CHA seeds were added to the stirred mixture. Theresulting gel was placed in a stirred autoclave with a total volume of1600 L. The autoclave was heated within 7 h to 170° C. The temperaturewas kept constant for 18 h. Afterwards the autoclave was cooled down toroom temperature. Then, the solids were separated by filtration andintensively washed until the wash-water had a pH of 7. Finally the solidwas dried for 10 hours at 120° C. The material was then calcined at 550°C. for 5 hours.

The characterization of the material via XRD confirmed the CHA-typeframework structure of the product and afforded an average crystal sizeof 118 nm and a crystallinity of 92%. The material displayed a BETsurface area of 654 m²/g, a pore volume of 1.09 cm³/g and a median porewidth of 0.68 nm. The elemental analysis prior to calcination showed 37wt-% Si, 2.8 wt-% Al, 12.1 wt-% C, 1.6 wt.-% N and 0.11 wt-% Na in thesample, thus affording an SiO₂:Al₂O₃ atomic ratio (SAR) of 25.

The IR-spectrum of the calcined sample is shown in FIG. 2, whereinamongst others absorption bands having maxima at 3,733 cm⁻¹ and 1,866cm⁻¹ may be seen, which display a ratio of maximum absorption of theformer to the latter of 1.35.

The particle size distribution of the calcined sample afforded a D10value of 0.40 μm, a D50 value of 0.58 μm, and a D90 value of 0.89 μm.

The ²⁹Si MAS NMR of the zeolitic material displays peaks at −104.2 and−110.5 ppm, wherein the integration of the peaks offers relativeintensities of 0.394 and 1 for the signals, respectively.

The ²⁷Al MAS NMR of the zeolitic material displays peaks at 58.5 and−2.7 ppm, wherein the integration of the peaks offers relativeintensities of 1 and 0.225 for the signals, respectively.

Comparative Example 1 Preparation of a Zeolitic Material having the CHAFramework Structure using Adamantyltrimethylammonium andTetramethylammonium

554.6 g 1-adamantyltrimethylammoniumhyroxide (20.44 wt.-% solution inH₂O) were mixed with 101.9 g of aluminiumtriisopropylate and 210.9 gtetramethylammonium hydroxide (25 wt-% solution in H₂O). Afterwards,1036.2 g of colloidal silica (LUDOX AS 40; 40 wt.-% colloidal solutionin H₂O) and 20.7 g of chabazite as seed crystals were added togetherwith 96.4 of distilled H₂O to the stirred mixture. The resulting gel wasplaced in a stirred autoclave with a total volume of 2.5 L. Theautoclave was heated within 7 h to 170° C. The temperature was keptconstant for 16 h. Afterwards the autoclave was cooled down to roomtemperature. Then, the solids were separated by filtration and intensivewashing with distilled water until the wash-water had a pH of 7. Finallythe solid was dried for 10 hours at 120° C. to afford 327 g of a solidproduct which was then calcined at 600° C. for 5 h to afford 296 g of awhite powder.

The characterization of the material via XRD confirmed the CHA-typeframework structure of the product and afforded an average crystal sizeof 119 nm and a crystallinity of 90%. The material displayed a BETsurface area of 644 m²/g, a pore volume of 0.72 cm³/g and a median porewidth of 0.18 nm. The elemental analysis of the calcined material showed42 wt-% Si, 3.1 wt-% Al, and 0.15 wt-% Na in the sample, thus affordingan SiO₂:Al₂O₃ atomic ratio (SAR) of 26.

The IR-spectrum of the calcined sample is shown in FIG. 3, whereinamongst others absorption bands having maxima at 3,732 cm⁻¹ and 1,869cm⁻¹ may be seen, which display a ratio of maximum absorption of theformer to the latter of 1.72.

The particle size distribution of the calcined sample afforded a D10value of 0.311 μm, a D50 value of 0.476 μm, and a D90 value of 0.766 μm.

The ²⁹Si MAS NMR of the zeolitic material displays peaks at −104.3 and−110.3 ppm, wherein the integration of the peaks offers relativeintensities of 0.311 and 1 for the signals, respectively.

The ²⁷Al MAS NMR of the zeolitic material displays peaks at 58.6 and−0.8 ppm, wherein the integration of the peaks offers relativeintensities of 1 and 0.1752 for the signals, respectively.

Comparative Example 2 Preparation of a Zeolitic Material having the CHAFramework Structure using Adamantyltrimethylammonium andTetramethylammonium

536.6 g 1-adamantyltrimethylammonium hyroxide (21.39 wt.-% solution inH₂O) were mixed with 103.9 g of aluminiumtriisopropylate and 213.6 gtetramethylammonium hydroxide (25 wt.-% solution in H₂O). Afterwards,1049.1 g of colloidal silica (LUDOX AS 40; 40 wt-% colloidal solution inH₂O) and 21.0 g of chabazite as seed crystals seeds were added togetherwith 97.6 g of distilled H₂O to the stirred mixture. The resulting gelwas placed in a stirred autoclave with a total volume of 2.5 L. Theautoclave was heated within 8 h to 170° C. The temperature was keptconstant for 24 h. Afterwards the autoclave was cooled down to roomtemperature. Then, the solids were separated by filtration and intensivewashing with distilled water until the wash-water had a pH of 7.Finally, the solid was dried for 10 hours at 120° C. and then calcinedat 600° C. for 5 h thus affording 457 g of a white powder.

The characterization of the material via XRD confirmed the CHA-typeframework structure of the product and afforded an average crystal sizeof 111 nm and a crystallinity of 92%. The material displayed a BETsurface area of 635 m²/g, a pore volume of 1.13 cm³/g and a median porewidth of 0.49 nm. The elemental analysis of the calcined material showed41 wt-% Si, 3.1 wt-% Al, and 0.11 wt-% Na in the sample, thus affordingan SiO₂:Al₂O₃ atomic ratio (SAR) of 26.

The IR-spectrum of the calcined sample is shown in FIG. 4, whereinamongst others absorption bands having maxima at 3,733 cm⁻¹ and 1,871cm⁻¹ may be seen, which display a ratio of maximum absorption of theformer to the latter of 1.59.

The particle size distribution of the calcined sample afforded a D10value of 0.257 μm, a D50 value of 0.578 μm, and a D90 value of 1.1 μm.

The ²⁹Si MAS NMR of the zeolitic material displays peaks at −104.6 and−110.6 ppm, wherein the integration of the peaks offers relativeintensities of 0.288 and 1 for the signals, respectively.

The ²⁷Al MAS NMR of the zeolitic material displays peaks at 58.7 and−3.5 ppm, wherein the integration of the peaks offers relativeintensities of 1 and 0.267 for the signals, respectively.

Comparative Example 3 Preparation of a Zeolitic Material having the CHAFramework Structure using Trimethylcyclohexylammonium

291.3 g trimethylcyclohexylammonium hydroxide (35.0 wt.-% in H₂O) aremixed with 42.88 g Al₂(SO₄)₃*18 H₂O and 160.84 ml 1 M aqueous NaOH.Afterwards 482.62 g of colloidal silica (LUDOX AS 40; colloidal SiO₂ ₄₀wt.-% in H₂O) are added to the stirred mixture. Finally 3.83 g ofNa-chabazite (having a silica-to-alumina ratio of 30) as seed crystalsare dispersed in the reaction mixture. The resulting gel is placed in asealed autoclave with a total volume of 2.5 L which is then heated to170° C. for 48 h. After cooling down to room temperature, the obtainedsodium containing a zeolite having the CHA framework structure isseparated by filtration and is washed with 2000 ml of distilled H₂Othree times. Afterwards, the material is dried for 10 h under air at120° C., resulting in 245.5 g of white powder. The product was thencalcined under air with a heating rate of 1 K/min to 550° C. for 5 h.

The characterization of the material via XRD confirmed the CHA-typeframework structure of the product and afforded an average crystal sizeof 150 nm and a crystallinity of 92%. The material displayed a BETsurface area of 627 m²/g. The elemental analysis of the calcinedmaterial showed 37.5 wt.-% Si, 1.6 wt.-% Al, and 0.1 wt.-% Na in thesample, thus affording an SiO₂:Al₂O₃ atomic ratio (SAR) of 45.

The IR-spectrum of the calcined sample is shown in FIG. 5, whereinamongst others absorption bands having maxima at 3,729 cm⁻¹ and 1,872cm⁻¹ may be seen, which display a ratio of maximum absorption of theformer to the latter of 1.46.

The particle size distribution of the calcined sample afforded a D10value of 0.49 μm, a D50 value of 0.637 μm, and a D90 value of 0.839 μm.

The ²⁹Si MAS NMR of the zeolitic material displays peaks at −103.8 and−110.4 ppm, wherein the integration of the peaks offers relativeintensities of 0.266 and 1 for the signals, respectively.

The ²⁷Al MAS NMR of the zeolitic material displays peaks at 57.5 and−0.0 ppm, wherein the integration of the peaks offers relativeintensities of 1 and 0.005 for the signals, respectively.

Comparative Example 4 Preparation of a Zeolitic Material having the CHAFramework Structure using Adamantyltrimethylammonium

174.6 g H₂O were stirred together with 478.8 g of a 20 wt.-%adamantyltrimethylammonium hydroxide solution in H₂O. 102.7 g NaOH (25wt.-% in H₂O) were added slowly under stirring. After 10 minutes 80.4 galuminiumtriisopropylate were dissolved in the reaction mixture followedby the addition of 963.4 g of colloidal silica (LUDOX AS 40; colloidalSiO₂ ₄₀ wt.-% in H₂O) after 60 minutes. Finally the reaction mixture isstirred for 30 min before it is placed into an autoclave, which isheated to 170° C. for 20 hours. After the autoclave was cooled to roomtemperature, the resulting dispersion was adjusted by means of a 10wt.-% HNO₃ solution in H₂O to a pH-value of 7. Afterwards to theresulting solid was filtered and washed with distilled H₂O until aconductivity of below 200 μS is reached. Afterwards the solid was firstdried at 120° C. for 10 h and then calcined under air at 600° C. for 6 hto afford 391 g of a white powder.

The characterization of the material via XRD confirmed the CHA-typeframework structure of the product and afforded an average crystal sizeof 55 nm and a crystallinity of 88%. The material displayed a BETsurface area of 615 m²/g, a pore volume of 1.59 cm³/g and a median porewidth of 0.88 nm. The elemental analysis of the calcined material showed40.5 wt.-% Si, 3.1 wt.-% Al, and 0.62 wt.-% Na in the sample, thusaffording an SiO₂:Al₂O₃ atomic ratio (SAR) of 31.

The IR-spectrum of the calcined sample is shown in FIG. 6, whereinamongst others absorption bands having maxima at 3,733 cm⁻¹ and 1,870cm⁻¹ may be seen, which display a ratio of maximum absorption of theformer to the latter of 2.43.

The particle size distribution of the calcined sample afforded a D10value of 34 nm, a D50 value of 0.28 μm, and a D90 value of 1.54 μm.

The ²⁹Si MAS NMR of the zeolitic material displays peaks at −104.0 and−110.5 ppm. The ²⁷Al MAS NMR of the zeolitic material displays a peak at58.1.

Comparative Example 5 Preparation of a Zeolitic Material having the CHAFramework Structure using Low Amounts of Trimethylcyclohexylammonium inCombination with Tetramethylammonium

Example 1 of WO 2011/064186 A1 was repeated with the exception thattrimethyl-1-adamantylammonium hydroxide was replaced bytrimethylcyclohexylammonium. More specifically, 267.0 gN,N,N-trimethylcyclohexylammoniumhydroxide (20 wt-% solution in H₂O)were mixed with 62.03 g of aluminiumtriisopropylate and 154.92 gtetramethylammoniumhydroxide (25 wt-% solution in H₂O). Afterwards,692.01 g LUDOX AS 40 (40 wt-% colloidal solution in H₂O) were addedtogether with 210 ml H₂O to the stirred mixture. The resulting gel wasplaced in a stirred autoclave with a total volume of 2.5 L. Theautoclave was heated within 7 h to 170° C. The temperature was keptconstant for 48 h. Afterwards the autoclave was cooled down to roomtemperature. Then, the solid was separated by filtration and washedintensively with H₂O until the wash-water had a pH of 7. Finally thesolid was dried for 10 hours at 120° C.

The characterization of the resulting product via XRD is displayed inFIG. 7 and revealed an amorphous material. For comparative purposes, theline pattern of the CHA type structure is indicated in the diffractogramof the amorphous material as a reference.

Accordingly, conducting the procedure of WO 2011/064186 A1 using thetrimethylcyclohexylammonium template instead of theN,N-trimethylcyclohexylammonium template taught therein as the structuredirecting agent does not afford a zeolitic material having the CHA-typeframework according to the present invention, but rather does not allowfor the production of any zeolitic material whatsoever.

Comparative Example 6 Preparation of a Boron-containing ZeoliticMaterial having the CHA Framework Structure using Low Amounts ofTrimethylcyclohexylammonium in Combination with Tetramethylammonium

Example 1 of EP 2325143 A2 was repeated with the exception thattrimethyl-1-adamantylammonium hydroxide was replaced bytrimethylcyclohexylammonium. More specifically, 577.9 g ofN,N,N-cyclohexyltrimethylammonium hydroxide (13.3 wt-% in H₂O), 203.8tetramethylammoniumhydroxide (25 wt-% solution in H₂O) and 163.4 ml H₂O(DI) were stirred in a beaker for 10 minutes. Afterwards 31 g boric acid(purity 99.6%) were added. The resulting mixture was stirred for another60 minutes. 999.6 g of an aqueous suspension of colloidal silica (LUDOXAS 40) were given into the reaction mixture followed by another stirringperiod of 20 minutes before 20 g of B-CHA seed crystals prepared inaccordance with Example A of EP 2325143 A2 were dispersed therein aswell. Finally the dispersion, was transferred into an autoclave. Thecrystallization was conducted at 160° C. for 72 h with a stirring rateof 200 rpm.

The obtained solid material was separated from the mother liquor byfiltration. Afterwards, the obtained filtercake was dried at 120° C. for240 minutes under air (heating rate within 30 minutes to 120° C.). Fromthe resulting white powder an X-ray diffractogramm was recorded.

The characterization of the resulting product via XRD is displayed inFIG. 8. An analysis of the pattern using a databank of XRD line patternsrevealed that the product consists of a mixture of numerous crystallinecompounds, of which not all could be identified and only a portionthereof even potentially displaying a diffraction pattern typical forthe CHA-type structure.

Accordingly, also when conducting the procedure of EP 2325143 A2 usingthe trimethylcyclohexylammonium template instead of theN,N-trimethylcyclohexylammonium template taught therein as the structuredirecting agent does not a pure zeolitic material having the CHA-typeframework according to the present invention, but rather leads to acomplex mixture of products of which only a minor portion might displaythe CHA-type framework structure. In particular, should said mixturecontain a zeolitic material having the CHA structure, it would not onlybe produced in a low yield but would furthermore—if at possible atall—require an extensive purification procedure for its isolation.

Example 4 SCR Catalyst Testing

For catalyst testing, the samples obtained in the examples andcomparative examples were subsequently ion-exchanged with ammonium andcopper for obtaining a zeolitic material having the CHA-type frameworkstructure with a copper loading in the range of from 2.2 to 2.9 wt.-%based on the total weight of the exchanged zeolite. The samples werethen extruded with polyethylene oxide and H₂O, and the extrudates werecalcined for 5 h at 540° C. under air. Afterwards the solids were sievedto a size of 0.5-1 mm. The obtained split fraction was aged for 6 h at850° C. under air with 10 vol-% H₂O. SCR tests on the extruded powderswere performed at 200, 300, and 450° C., respectively, using a gasstream with 500 ppm NO, 500 ppm NH₃, 5% H₂O, 10% O₂, balance N₂, using agas hourly space velocity GHSV of 80,000 h⁻¹.

In addition to the catalytic testing performed on the powder (“PowderTest”), the ion-exchanged samples were additionally coated on monoliths(“Core Test”) at a washcoat loading of 2.1 g/in³. The washcoated sampleswere then aged at 750° C. for 5 h in air with 10% H₂O. The SCR tests onthe washcoated samples were performed at 200 and 600° C., respectively,using a gas stream with 500 ppm NO, 500 ppm NH₃, 5% H₂O, 10% O₂ (asair), balance N₂, using a gas hourly space velocity GHSV of 80,000 h⁻¹.The results from the testing of the powder and wash-coat samples aredisplayed in Table 1.

TABLE 1 Results from SCR testing. Comp. Comp. Comp. Comp. Ex. 1 Ex. 2Ex. 3 Ex. 1 Ex. 2 Ex. 3 Ex. 4 Cu [wt-%] 2.3 2.5 2.2 2.7 2.9 2.5 2.3 2.52.3 Powder NO_(x) conversion 71 75 85 n.a. n.a. 77 67 82 75 Test [%] at200° C. NO_(x) conversion 80 84 89 n.a. n.a. 82 69 96 84 [%] at 300° C.NO_(x) conversion 78 80 85 n.a. n.a. 76 69 77 74 [%] at 450° C. CoreNO_(x) conversion n.a. 67 65 73 75 n.a. 71 64 62 Test [%] at 200° C.NO_(x) conversion n.a. 83 88 76 77 n.a. 78 65 67 [%] at 600° C.

Thus, as may be taken from Table 1, the results obtained using theinventive examples clearly show that the zeolitic material obtainedaccording to the inventive examples of which the synthesis employs aspecific combination of a tetraalkylammonium cation and acycloalkylammonium cation display an improved performance in SCRcatalysis, in particular at higher temperatures. This is particularlyapparent when comparing the results obtained in the “Core Test” whichwere performed on coated monoliths as typically used in the art for theabatement of NO_(x) emissions such as in the treatment of automotiveexhaust gas. Thus, although the inventive catalysts with similar oridentical copper loadings display comparable conversion rates at lowertemperatures, said conversion increases to a surprising extent uponraising the temperature to clearly surpass the catalysts obtainedaccording to the comparative examples at 600° C. The effect observed forthe inventive catalysts is highly unexpected in view of the fact thatalthough a certain improvement in the conversion of NO_(x) may beobserved for Comparative Examples 1 and 2 which are also obtained usinga tetraalkylammonium cation however in combination with a structuredirecting agent well known in the art, said increase in activity isclearly inferior to the surge in activity observed for the inventivecatalysts according to Examples 2 and 3. Same applies accordingly whencomparing said considerable increase in activity with the resultsobtained for the materials obtained without a tetraalkylammonium cationin addition to the structure directing agent in Comparative Examples 3and 4. Consequently, it has been clearly demonstrated by the elaboratecomparative testing performed for the present application that theunexpected properties of the inventive materials and in particular theiroutstanding catalytic performance in SCR is the result of a synergeticeffect observed for a highly specific combination of a particularstructure directing agent with a tetraalkylammonium cation which may notbe achieved by a particular structure directing agent alone, nor by acombination of a different structure directing agant than the one usedin the inventive process with a tetraalkylammonium cation.

Accordingly, the zeolitic material having a CHA-type framework providedby the present invention clearly distiguishes itself from zeoliticmaterials as may for example be obtained according to the art not onlyin view of their unique physical characteristics but far more due totheir highly unexpected chemical properties in particular in theconversion of NO_(x) by selective catalytic reduction such as to makethem particularly promising candidates for highly efficient SCRcatalysts. This also applies in view of their highly cost-effectiveproduction made possible by the particularly fast synthetic procedure ofthe present invention employing inexpensive structure directing agents.

1.-15. (canceled)
 16. A process for the preparation of a zeoliticmaterial having a CHA-type framework structure comprising SiO₂ andAl₂O₃, wherein said process comprises the steps of: (1) providing amixture comprising one or more sources for SiO₂, one or more sources forAl₂O₃, one or more tetramethylammonium compounds, and one or moreN,N,N-trimethyl-cyclohexylammonium compounds as structure directingagent; (2) crystallizing the mixture obtained in step (1) for obtainingthe zeolitic material having a CHA-type framework structure; wherein themolar ratio of tetramethylammonium compounds toN,N,N-trimethylcyclohexylammonium compounds is comprised in the rangefrom 0.45 to 0.65.
 17. The process of claim 16, wherein thecrystallization in step (2) is conducted under solvothermal conditions.18. The process of claim 16, wherein the mixture provided in step (1)does not contain any substantial amount of a trimethyl benzyl ammoniumcontaining compound.
 19. The process of claim 16, wherein the mixtureprovided in step (1) further comprises seed crystals.
 20. A syntheticzeolitic material having a CHA-type framework structure prepared by theprocess of claim
 16. 21. A synthetic zeolitic material having a CHA-typeframework structure, wherein the CHA-type framework structure comprisesSiO₂ and Al₂O₃, and wherein the IR-spectrum of the zeolitic materialincludes: a first absorption hand (B1) in the range of from 3,720 to3,740 cm⁻¹; and a second absorption band (B2) in the range of from 1,850to 1,890 cm⁻¹; wherein the ratio of the maximum absorbance of the firstabsorption band to the second absorption band B1:B2 is in the range offrom 0.5 to 1.55.
 22. The zeolitic material of claim 21, wherein theparticle size D10 of the zeolitic material is comprised in the range offrom 400 to 2500 nm.
 23. The zeolitic material of claim 21, wherein theaverage particle size D50 of the zeolitic material is comprised in therange of from 600 to 3500 nm.
 24. The zeolitic material of claim 21,wherein the particle size D90 of the zeolitic material is comprised inthe range of from 1200 to 4,500 nm.
 25. The zeolitic material of claim21, wherein the CHA-type framework contains 5 wt-% or less of theelements P and/or As based on 100 wt-% a of SiO₂ contained in theframework structure.
 26. The zeolitic material of claim 21, wherein the²⁹Si MAS NMR of the zeolitic material includes: a first peak (P′1) inthe range of from −102.0 to −106.0 ppm; and a second peak (P′2) in therange of from −108.0 to −112.5 ppm, wherein the integration of the firstand second peaks in the ²⁹Si MAS NMR of the zeolitic material offers aratio of the integration values P′1:P′2 comprised in the range of from0.05 to 0.90.
 27. The zeolitic material of claim 21, wherein theSiO₂:Al₂O₃ molar ratio ranges from 4 to
 200. 28. A synthetic zeoliticmaterial having a CHA-type framework structure, wherein the CHA-typeframework structure comprises SiO₂ and Al₂O₃, and wherein theIR-spectrum of the zeolitic material includes: a first absorption band(B1) in the range of from 3,720 to 3,740 cm⁻¹; and a second absorptionband (B2) in the range of from 1,850 to 1,890 cm⁻¹; wherein the ratio ofthe maximum absorbance of the first absorption band to the secondabsorption band B1:B2 is in the range of from 0.5 to 1.55; wherein theparticle size D10 of the zeolitic material is in a range of from 400 to2500 nm, the average particle size D50 of the zeolitic material is in arange of from 600 to 3500 nm, and the particle size D90 of the zeoliticmaterial is in a range of from 1200 to 4,500 nm, and a ²⁹Si MAS NMRspectrum of the zeolitic material includes: a first peak (P′1) in therange of from −102.0 to −106.0 ppm; and a second peak (P′2) in the rangeof from −108.0 to −112.5 ppm, wherein the integration of the first andsecond peaks in the ²⁹Si MAS NMR of the zeolitic material offers a ratioof the integration values P′1:P′2 comprised in the range of from 0.05 to0.90.
 29. The synthetic zeolitic material of claim 21, wherein thematerial is an adsorbent material, an ion-exchange material, a catalystor a catalyst support.